First, Zola Jesus singing "Vessel." All the mixing in her songs results in not-my-cuppa-tea music, since you can't really hear her awesome voice. But the video is cool, and I'm sure others out there will love her - mainly, the industrial rock crowd.
First Aid Kit is a group Spousal Unit discovered. They're a couple of Swedish sisters with an awesome folk sound and great voices. The vocal syncopation is especially unusual in this song, but it works out very well.
Last, Lucy Rose, a self-taught guitarist, sings "Middle of the Bed." I'm impressed that she can sing so fast and well at once, and there's something about the song that makes it sound incredibly smooth and deliriously choppy - in a good way.
Another one I love is Danielle Ate the Sandwich - yes, that's the name of the band. Her song "17 and 53" is sad, but beautiful.