Toy Biz. Hasbro, Legends, Movie Figs, exclusives... it doesn't matter.
BAF figs themselves don't count.
I was looking at my Marvel shelf and it seems a few new ones are really standing out now that I know more about the characters:
1. Long Haired Winter Solider: This is probably the most detailed realistic ML/6" figure I own. Everything aspect of this sculpt is amazing. He looks pissed and ready to get the job done.
2. Marvel Face-Off Masked Captain America: I don't care how old it is, to me, it is still THE best Steve Rogers Cap there is. The unmasked version is equally as cool.
3. Toy Biz Astonishing X-Men Wolverine Unmasked \Version: I don't know why, but I have really become a HUGE Wolverine fan these past 2 years and never realized I had this gem in my collection as well as a 12" version. It is perfect in every way.
4. Hasbro 6" Fantomex: I initially bought him because he just looked cool and reminded me of Storm Shadow..now I really know the character and like him that much more.
5. Toy Biz Spiderman Classics Hobgoblin: I don't think this figure will ever cease to be a favorite of mine. It's a fantastic representation of the Amazing #238 debut.
Runner-up would Hasbro's Bucky Cap figure. It looks awesome, but I actually prefer the look of the 3 3/4" more as it just seems more realistic in that scale with regards to the face sculpt.
The 2pk version of Winter Solider is an example of how good Hasbro face/head sculpts can be if they focus on making it happen.
You just took 3 of them off my list when you said no BAFs (Galactus, MODOK, and Arnim Zola)
Anyway, I'm gonna bend the rules a little and make the distinction between Toy Biz and Hasbro...just because.
Toy Biz
Hasbro
Toybiz: Deadpool
Marvel Select: Avengers Movie Hulk
Hasbro: Galactus
Hasbro: Fin Fang Foom
Marvel Universe: Adam Warlock
(Because I love the character and the figure is decent. I want a repaint though in not so shiny colors.)
Runner Up: Marvel Select Thanos