Watch a videosong by Pomplamoose and you'll be as equally charmed by Nataly Dawn's doe eyes and silky voice as you are with Jack Conte's mastery of instruments ranging from a xylophone to a toy piano. This is how the romantically-tied Stanford grads took off this fall, with a string of high-energy original songs and viral YouTube covers. We caught up with Nataly to find out more.

• The name is derived from the French world for "grapefruit."

What is a videosong?

It's a medium that Jack came up with out of the desire to create authentic music and something he could quickly upload to YouTube. There are two rules. What you see is what you hear, so there's no dubbing. And then if you hear it, at some point you will see it—there are no hidden sounds.

With YouTube, iTunes and Twitter, is there a need for record labels anymore?

There'll always be Lady Gagas in the world that need the infrastructure of a major label to do what they do. But, if you're consistent and creative, there are so many outlets now to reach an audience without giving a company the rights to your music or releasing creative control.

Dream collaboration?

I'd love to have Mark Ronson produce a Pomplamoose album. I love his arrangements—the punchy horns and the beats are incredible.