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If you know Kaki King, you know her as a guitar player. A special one. A rare breed of genreless six-string (rather than five-button) Guitar Hero: young, female, Southern, and slight of stature. Her facility has been freshly flaunted and recently rewarded by no less than a Golden Globe nomination for her soundtrack work on Sean Penn's Into the Wild; more tangibly, she received a "sweaty, shirtless hug" from Dave Grohl after their duet on the recent Foo Fighters track, "Ballad of the Beaconsfield Miners."

Yes, King's talent manifests itself both aurally and visually. Particularly on those two-handed "tappy" numbers, wherein, like a discordant disciple of Smokey the Bear, she figuratively sets her guitar alight while physically smothering that same instrument with frequent and furious hand pats, as if trying to put out a fire without the benefit of blanket or extinguisher. And yet despite these fingers of frenzy (honed by her years as a teenage percussionist), on disc, King's compositions soar lightly, like a balloon peering down on some new-age/jazz hybrid.

But even if you've heard (or seen) King's guitar work, you are likely unacquainted with her voice. Only four of the 11 songs on her new Dreaming of Revenge contain vocals, but even that small percentage is a meaningful increase from her 2003 debut, the fully instrumental Everybody Loves You. Like that of, say, Jill Sobule or Juliana Hatfield, King's not-oft-heard voice is near-childlike in its high-pitched guilelessness. So it's not surprising that, when we meet at the confluence of the L, F, and V lines below 14th Street and Sixth Avenue to re-create a session from King's days of busking past, she offers a cookie. And not just any shortbread, either. No, the multiple musical threat arrives with a selection of black-and-white cookies replete with Seinfeld-ian symbolism—you know, the undulating universality of New York City. These proffered pieces of frosted baked goods are a foreshadowing as well, for, as we will learn, they resolutely represent King's munificence of spirit.

Not that there's anything wrong with that.

"Busking," she says, "really came out of . . . it totally dealt with 9/11. I started busking because it really was something to just . . . do. Like, how does one spend their time?"

When the planes hit, King was just short of completing her studies at NYU. In fact, her colloquium—sort of an oral defense in her field of study, Music and Aesthetic Philosophy ("What I studied was a lot of literature, a lot of philosophical text, and a lot of music")—was scheduled for September 12, 2001. "Instead of having, you know, the future ahead of me, and life is beautiful, I'm in New York going, 'What . . . am . . . I . . . doing?' And we were all like that."

Yes, we were.

Within the most unique aftermath in the city's history—a period defined by shock and suspicion, reaching out and reassessment—Kaki King took her guitar and headed toward the subway.

"It was a hell of a lot better than sitting at home," she says. "The following weeks, it was terrible being around, because all the photographs of people were everywhere, on every bus stop and everything. And you realized pretty soon that those people were all dead. So it honestly just gave me a healthy way to spend my time."

There were other benefits as well. The mettle of the moment, combined with the uncommon sight of a sprightly Southern female barely able to restrain a definitively dramatic talent, added up to more than a little pocket change at a time when King was technically unemployed.

This, of course, was all before Atlanta native and NYU graduate Kaki King became "Kaki King, recording artist." And so, over an eight-month period, from the autumn of 2001 into the following spring, she played through a roughly 12-song repertoire (plenty for a guitarist who starts and stops in time with the trains as they enter and exit the station)—a Martin Simpson cover, a Preston Reed cover, her own material. Instrumentals like "Night After Sidewalk," "Happy as a Dead Pig in the Sunshine," and "Close Your Eyes & You'll Burst into Flames" were all performed underneath 14th and Sixth in front of a transient and transiting audience. And each of those expansively titled tunes found a home on King's first album.

"A lot of it," she says, "was sort of my training ground to get really good at those songs."

Soon enough, King was performing with the Blue Man Group; then came a regular gig at the Knitting Factory and a recording contract. And yet those underground sessions brought her something else. Something, as saccharine as it may sound, even more important than the first firm footsteps of what would become her career.

"I would play, and people would thank me," she says. "Or they would write me a note. And I don't think that would happen now. And for me, being able to just play music and be in the world . . . having a shared experience during that time was really very important. I felt like people really appreciated having someone just playing music—like a generosity of listening. It was a very nice experience, but a poignant one at the same time."

Kaki King plays the Bowery Ballroom April 9, boweryballroom.com.

To see footage of Kaki performing at the 14th and Sixth subway platform, see Rob Trucks's Possibly 4th Street column here.