ROLA, then TLC, then TOD... That's my order right now, but I don't really know why. I guess I found Indy's dad a good character, I liked Sallah's return, I wasn't really bothered by the Marcus Brody character, and the villains were no better/worse to me than Rene Belloq and Col. Dietrich (am I getting his name right?) and Toht...
I think they went the extra mile with Vogel to make sure he OOZED Nazis though, compared to Dietrich and co. from Raiders... Donovan I dug because of the double-cross like Scott said, but really Belloq delivered cooler lines, I agree with that too.
I liked Raiders' story more though, in general.
I'm really hoping this line goes obscure... I know, I know, it's probably wishful thinking, but I'd be down for a ton of obscurity from Raiders. The mechanic is almost a main character compared to my list.
I want the flying wing pilot, Cairo Gestapo agents, Belloq in jungle duds, Indy's pilot friend, the captain of the U-Boat (was he played by Michael Sheard? Or am I not remembering correctly?), the freighter pirate captain, and all kinds of crap. I'd love figures like that, but I know there's probably not as much hope.
I think Temple has less figure selection than any of them... Club Obi-Wan I think would be getting obscure, but possible... Once you're in India though, your choices become a bit more limited it seems, and you've got the big Thugee, a generic small one, Indy damaged, Indy normal, Willie, Short round... Stuff just seems to get limited though.
The Last Crusade seems to really have the better character selection overall, at least to me anyway.