Yeah, Scott's lists are pretty good. I'd say She-Hulk, to me, is the most glaring omission in the Legends lineup so far. I'd like the following too (as well as a few I'm likely forgetting):
She-Hulk
Quicksilver
The Blob
Mole Man
US Agent
Black Bolt
There are probably others I might pick up too, but those are a few I wouldn't mind seeing. Of course, there are always wish lists for the rest of Spidey's universe (Mary Jane, Aunt May, J.J. Jameson) - but those are unlikely, and if so, we'll leave those for SMC.
Looking at the Marvel Legends (and the accompanying Classics line) throughout the 15+ series, its really amazing all the characters that have been covered. I certainly didn't end up getting the majority of the figures, but for those that did I can't imagine what type of a Marvel Universe set up you could have gotten. I've always been a Star Wars fan/collector first and foremost, but this line is really a Marvel fan's dream come true I think. I couldn't imagine having a lineup like this as a kid when I was reading comics, and now getting back into comics again - its pretty cool. Anyways, like both of you have mentioned, there isn't much left that I necessarily need. Just a few figures here and there, but for the most part nothing I can't live without. That said, I'll probably end up picking more than I think now, depending on how expansive the Star Wars line is next year again.