Out of the albums/releases I have, my fave of each has to be:
Big Bang [Float]
One Brick [Labor Days]
Holy Smokes [Fast Cars...]
Mars Attacks [Bazooka Tooth]
Nickle Plated Pockets [Daylight]
The Harbor Is Yours [None Shall Pass]
Edit:
Honestly I can probably feel good about changing that list a hundred times. Those are just the first ones I think of when I consider the albums. There are very few of his songs I actually don't like a lot.
I still need to get Music For Earthworms though. I've heard it but I don't have it.