Sitting shoulder to shoulder on high stools, in front of a handful of microphones at Electric Lady Studios in New York, singer Chris and guitarist Rich Robinson of the Black Crowes look nothing like kin and act even less like bandmates.

The Georgia-born brothers are recording a dozen numbers as a duo, unplugged, a few weeks before the release of their band's new album, Warpaint, on the Crowes' own Silver Arrow label. Eleven tracks of brawny Southern rock and psychedelic R&B ecstasy, Warpaint is the Crowes' first studio album in seven years and their first since the Robinsons reunited in 2005 after a tense three-year split. Like the Kinks' Ray and Dave Davies and the Gallagher brothers of Oasis, Chris and Rich — who were teenagers when they formed the earliest version of the Crowes in Atlanta in the mid-Eighties — are as famous for their arguments and outright combat as for anything else, including their vintage-rock aesthetics, live-show lightning and multiplatinum breakthrough records, 1990's Shake Your Money Maker and 1992's The Southern Harmony and Musical Companion. And at Electric Lady, whenever they are between songs, the Robinsons are a compelling study in potentially explosive opposites.

Chris, 41, is a hippie whirlwind with a pointed Jesus-like beard, lanky dark-brown hair and a ski-pole physique. He is always in some kind of motion — tapping a foot, pacing the floor, lighting a hand-rolled smoke — and he talks at dizzying velocity in a bouncy Southern drawl punctuated by a sharp chuckle whenever he finds something funny, which is often.

Next to that verve, Rich, 38, is still water. Clean-shaven, with boyish features and a stevedore's build, he speaks as little as necessary — in a deep, certain voice with no obvious Dixie in it — and smiles even less, especially when Chris is at his elbow, in hypergear. "You should write this down," Chris says, cackling, when Rich stumbles at the start of one song, trying to recall a guitar part. "The one who doesn't smoke weed doesn't remember anything!" Chris turns to Rich and pats him on the shoulder. "That was just a little witticism at your expense, little brother." Rich stares down at his guitar as if he hasn't heard or felt a thing.

When the Robinsons were younger, that was enough to start real trouble. Pete Angelus, who has managed the Black Crowes since 1989, remembers their first professional photo session: "I turn my back to talk to the photographer. Within three minutes, a fistfight broke out. It was shocking even to me. How could something escalate to that level in such a small amount of time?" Even now, managing the brothers, Angelus says, "is not a matter of having a conversation every week. You're in the middle of helping them communicate on a daily basis."

For Chris, the grief is worth it. "We built this locomotive," he says, explaining why he returned to the band after three years. "It's sitting out in the field, with daisies growing through it. Let's shine it up! The work was important to us. The work was the only fucking interesting thing going on."

And when the music begins at Electric Lady, Chris and Rich are a perfect match, blood-bound partners in their vocal-guitar rapport and the country-soul righteousness of their songwriting. In a bare-bones version of "Walk Believer Walk," a greasy-gospel stomp on Warpaint, Chris' grainy howl soars and dives in acid-church rapture as Rich rides shotgun on dobro, in cutting bottleneck runs. In an old Crowes song, "Wyoming and Me," Rich hovers alongside Chris' plaintive bark in bright, empathic harmony.

And when they cover "Torn and Frayed," the great road-life song from the Rolling Stones' Exile on Main Street, the Robinsons sound like they are reliving all of the good and bad they've known, as partners and family. "You think he's bad/He thinks you're mad," Chris and Rich sing together, on their way to a chorus that explains why, despite every difference, they are still in the Black Crowes: "As long as the guitar plays/Let it steal your heart away."

"There is something about their shared genes," says Crowes bassist Sven Pipien, 40, who has known the Robinsons since he and they were in rival high school bands in Atlanta. "It's very difficult to sing with Chris — he changes his inflections so much. But Rich knows his brother. I've known Chris long enough to sing with him, but not as innately as Rich does."

"It's not correct singing," Chris declares cheerfully in his Soho hotel room the day after the Electric Lady session. "We are hardly articulate harmony singers. But it's in that close-harmony tradition of the Louvins and the Everlys — the thing that makes brothers singing together so special." Chris and Rich's father, Stan, was a pop star himself for a moment in the late Fifties — his 1959 single "Boom-A-Dip-Dip" went to Number 83 in Billboard — and Chris remembers him as a taskmaster in living-room hootenannies. "When we were kids and wanted to join in, if you didn't sing the right harmony," Chris says, laughing, "my dad would tell you to shut up."