My personal favorite is Guardian Heroes. It's like a really deep version of Final Fight, with lots of selectable characters and branching paths.
I also recommend:
Virtua Fighter 2
Panzer Dragoon 1 and 2
Panzer Dragoon Saga
X-Men vs Street Fighter (you will want a ram cart for this)
Die Hard Arcade
I never used the AR 4 in 1 so I can't really say anything about it