Is it? He didn't produce Come On Pilgrim, which has the same "pre-Dolittle" sound. I don't know that the "in the room with the band playing live" effect jumps out at me about Surfer Rosa --- also my favorite Pixies album.

Pod or Rid of Me would be my Albini production picks, if only for how different they each are to their immediate successor albums. If I can't pick an actual Albini album, that is (my pick would be At Action Park).