“Take a good look around you,” grins Cee Lo Green as he leans back in his chair, which sits on the patio of a mountain lodge-style house deep in a Georgia forest. Ahead of him is a swimming pool where the water is the coolest blue, set in a clearing among trees bathed in glorious late-summer sunshine. “You think I got anything to complain about?”

Above him, inside the glass-walled living room, Green’s new backing band – an all-woman five-piece – are getting ready for this afternoon’s rehearsal. The band is part of the concept he’s building around his third solo album, The Lady Killer, a set of love songs with a summery 60s vibe that recast the big, bald, heavily tattooed Cee Lo as a special agent of pop-soul heartbreak, ready to trot the globe with his private army of guitar-toting Bond girls.

Green’s 007 has his Q to supply him with hi-tech weaponry, too – the singer-songwriter Bruno Mars, with whom he has concocted one of the standout pop moments of the year: the album’s first single, Fuck You. The track, in which Green berates an ex who’s ditched him for someone with more money, became a viral hit last month, picking up more than 2m YouTube plays in just its first weekend online. It is expected to follow Mars’s Just the Way You Are to the top of the charts, and give Green his first solo No 1 in Britain when it’s released on Monday.

It’s not just the expletive in the title and hook – changed to Forget in the radio version – that have attracted attention. Green’s mix of self-deprecating humour and indignation, pitched just the right side of petulance, give the song a breadth of appeal that would have seemed unlikely to anyone who had heard only the title.

“It wouldn’t work for just anyone,” he says, with a contented smile. “Some people have misconstrued Bruno’s contribution as him writing the song for me. If he knew the song was gonna be a big hit, he’d-a wrote it for himself! Nobody else would’ve got away with it but me. Look at me! I’m not ideal image-wise, I don’t think. I get a chance to stand out there and redefine what’s doable. I am a fuck you – that’s why the song works.”

Between the song’s infectious, playful effortlessness and his evident self-belief, Green gives an impression of comfortable confidence, but that’s a front he has worked hard to cultivate. A divorced father of three (he has a biological son and is the adoptive father of his ex-wife’s two daughters), he was born Thomas DeCarlo Burton in Atlanta in 1975, to Baptist preacher parents. His father died when Green was two; he later changed his surname to Callaway, his mother’s maiden name. As a teenager with considerable capacity for anger, he became involved in gangs, drugs and violence. “Fortunately, music intervened in my life,” he says, “and gave me something to focus on.”

At elementary school he’d made friends with a fellow outsider, André Benjamin, and almost became a member when Benjamin and Antwan Patton formed Outkast. By then, they were all part of the extended Dungeon Family, which coalesced around the Atlanta production outfit Organized Noize, and Green joined the band Goodie Mob. Their 1995 debut album, Soul Food, included the track Dirty South, which gave a name to the nascent southern hip-hop scene. After recording but before release, Green’s mother died; she had been disabled by a car crash two years earlier and, as Green sees it, let go of life after tiring of immobility.

Though Cee Lo was primarily a rapper, one of the Organized members had heard his distinctive singing voice and asked him to do backing vocals on a session with the Atlanta group TLC in 1994. The song, Waterfalls, became the first No 1 he appeared on. More than a decade later, he made chart history in the UK when Gnarls Barkley, the duo he established with the producer Danger Mouse, were the first group to have a chart-topper on download sales alone: that song, Crazy, was the biggest-selling single in Britain in 2006.

Green calls Gnarls Barkley “a freak occurrence, a total eclipse of the sun: it’ll happen, but not every day”. His lyrics for the duo’s two albums have been his most introspective and confessional – Crazy may have become an anthem, but it’s a song about the terror of mental instability; She Knows was him dealing, years after the fact, with his mother’s death.

“That song is about possession,” he says. “My mother, being a prized possession of mine, and vice versa; and then me being possessed by her spirit. I understood her wanting to move on – not give up, but move on. She could’ve died immediately in the accident, and I can’t say that I would have reacted as positively to that. But to watch her suffer for a few years straight – and watchin’ her bein’ brave enough to make a sound decision to move on – I now believe that that was merciful on me.”

He intends more Gnarls Barkley albums, but making them clearly takes a toll; the Lady Killer is his way of escaping from the emotional intensity. Danger Mouse’s lack of a lighter outlet, though – his recent work has included Dark Night of the Soul, with the late Sparklehorse leader Mark Linkous and film director David Lynch – gives Green pause for thought.

“I don’t really have an in-depth opinion about anything Danger does outside [Gnarls],” he ponders, “but I feel the mood of things he’s done, and it concerns me about a real part of him that I do know. I know he’s not pretending – that’s truly his mood, and it’s very dark and melancholy and bitter and sad and detached and disturbed. But I also know a lighter side of him that he will share with me, but he won’t share with the world. Danger Mouse is Danger Mouse 24 hours a day – I couldn’t bear the thought of people bein’ so utterly convinced that I’m Gnarls Barkley 24 hours a day. I needed a break from it.”

Green has had extensive success with collaborations: before Crazy came out, Don’t Cha, a song he wrote and produced, was a hit for the Pussycat Dolls. Yet when he makes his own music, fewer people pay attention. His first two solo albums, released between Goodie’s dissolution in the early 2000s and the inception of Gnarls Barkley in 2005, were commercial failures. Musically expansive, thematically rich, daring in terms of the vulnerability he revealed and the acuity of his insight into art, life, politics and the human condition, both of them – Cee Lo Green and His Perfect Imperfections and Cee Lo Green … Is the Soul Machine – are masterpieces, exquisite records by an artist seemingly oblivious to creative boundaries. Their failure to connect with larger audiences seems to gnaw at him.

He has spent three years on The Lady Killer, recording close to 70 songs, reining in the eccentricities of the two predecessors, swapping the emotional evisceration of his Gnarls Barkley material for love songs. And he has opted to work with his label and management to assemble what they collectively believe is the record that will make him a household name, rather than release another album he might have felt better represented every aspect of his creative self.

“I could’ve said, ‘This is the album, take it or leave it,’ but I don’t think that’s the right attitude to have right now,” he admits. “For too long I’ve been underground and underdog, and I need to be seen as the thing to do: ‘This is the direction to go in – follow this man.’ I think I’m needed – as an artist, as an individual, as an entity, an enigma, an exhibitionist, an entertainer; as an alternative. So we sat down and weighed up the pros and cons, because you don’t seal a deal with one single solitary opinion. Tolerance, compromise, understanding, acceptance, patience – I want those all to be very sharp tools in my shed.”

The record isn’t finished yet (Green postponed a London gig last Monday to complete recording). But he has the follow-up to Fuck You ready and waiting. You Don’t Shock Me Any More is a breezy slice of retro soul-pop with a 21st-century attitudinal twist; a pastiche of 70s library and gameshow music with a delicious sax solo by Goodie Mob’s Khujo and a knowing lyric that’s part love song, part attack on celebrity culture. There’s only one problem: it didn’t make the committee’s cut for the album, so Green has released it, for free, on a mixtape called Stray Bullets.

“No one had anything to do with Stray Bullets but me,” he says. “I just needed a moment of clarity to have some fun. It’s a completely gratifying, exhilarating act of art. With Lady Killer, I had to take all those other things into consideration, because I wanna be a professional, but the growing pains hurt a bit. I’m not allowed to be as liberal as I would like to be, you know? I’d do a lot more damage if I could! So, I know I shouldn’t say this, but I’ve got to: personally, I like Stray Bullets better. But I hope you don’t think I’m insulting Lady Killer – I’m not. They’re all still pretty great songs.”

There aren’t many musicians who would consider releasing a single called Fuck You to be selling out in some way. But for Green, this is as safe as it gets. He just hopes he’s done enough to reap the rewards he feels he’s already earned several times over.

“I’m an artist, and I like the risk – I’m not in it for the sure things. I like the want, the need, the desire to live and die by it – it’s that serious for me. But on the other hand, someone like myself should survive. This should not be a kamikaze mission.”

Fuck You is released Monday on Elektra; The Lady Killer follows in November.