Sweet Sister Ray, Move Back or any other version of the Columbus 1966 show and " Guess I'm Falling in Love" are the only ones I can think of from the sixties. Most of the '93 europe tour was recorded as well.
Just remembered,Caught Between the Twisted Stars is probably your best bet. It also has the Poor Richard songs(Venus, Heroin) w/ Cale singing as well as some stuff from the Dom if I'm not mistaken