I've always loved or appreciated at least half or more of the songs on VU&N to death, but only that much. There's a few nondescript tunes in there for me.
Off & Nico album I like "European Son" the best, almost entirely for the bassline and the insane lead guitar work.
Favorite Velvets album is White Light/White Heat though---tossup for favorite VU song ever is very possibly between "Lady Godiva's Operation" and "Sister Ray".