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The big ones are the 33% chance of teleporting to the angel room at 6 plays, the 33% chance of spawning an angel item at 7 plays, and the 50/50 of 7 soul hearts or 30 pennies at 10 plays.
If you have the ability to reroll/void/etc the key pieces, you get value out of fighting the angels, too. If not, you can exit the room and they despawn.
Edit: You should also check curse rooms if you can spare the HP. The damage does not count for devil/angel room chance and while the contents are sometimes crap, they can also be great.