#1-#367

Best Character: Spider-Man, he is so much better then everyone else! I sometimes find it hard to belive that his mags are from the same time as all the other.
Best Villain: probably my childhood memories/knowledge of him.. but i have to go with Green Goblin. Always loved him!
Best Group: The Avengers, im kinda disapointed about all the groups at this time. but i find the avengers better then the rest (even though FF have had the best arc so far (inhumans + galactus).
Worst Character: i would say antman/giantman.. but since he "dosn't exist" as the ant/giant man anymore, i'll say DD.
Worst Villain: Stilt-man!
Worst Group: The Enforcers. lasso+strongman+smallman = boring!

ok, now i have come to the 70's, so i take a new look on my picks.

Best char: still spider-man!
best villain: i still love the Goblin, but i find Galactus to be the best villain from the 60's
best group: hmm.. i think i have to change my pick to FF
worst char: Rick Jones! when he started playing bucky it was just BAD!
worst villain: can i just say 75% of the DD villains? if i have to pick one.. probably still stilt-man, i cant understand why they keep bringing him back!
worst group: the ani-men

I put up acouple new categories:

most improved char from the 60's: The hulk. The start was AWEFUL! but he has realy grown on me.
most improved villain: Magneto
most improved group: The x-men, the first issues was hard to get through, but they have improved and finished strong in the 60's
the char that has worsen most: Nick fury. I liked his mag in the start, but that changed realy fast for me. and now i have to force myself to read his mag.
the groupe that has worsen most: not sure...
the villain that has worsen most: the puppet master? not that he was that good to start with, but he still manage to get even worse troughout the 60's.

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Issues to read till I get to Giant-Size X-Men #1 = 447

#1-#580

Best Character: Spider-Man. He's the guy that gets the most sympathy from me. He is the most natural character and I like that they're focusing on his non superhero life.
Best Villain: Galactus. He's not actually the villain, he's just doing what he must. The attempts are making him the evil character, but so far his stuff was really epic
Best Group: Back and forth between the Shield and FF. I think I'll go with FF
Worst Character: I really like Daredevil as a character. The problem is his storylines, so I'm not gonna pick him. Namor is the guy I like the least so far
Worst Villain: A lot and I mean A LOT of them. Animal people are still my #1 nightmare along with Paste-Pot...oh yeah, Trapster. Also I hated Thinker and Human top
Worst Group: X-men. Can't wait for their next installation

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For the entirety of the 60's

Best Character: Spider-Man. There's really no competition here. Peter is the only one who I thought had meaningful character development, and he's by far the most easily identified with.

Worst Character: Henry Pym. Might as well have named him Blandy McBlanderton for all the development and character he had in the 60's. Single biggest moment for him at this point was the death of that one ant, y'know that one that only appeared in the story it died in and has never been mentioned since.

Best Group: Purely from a character perspective I've gotta go with the Avengers. FF should probably win overall, but in the late 60's the Avengers really turned the character stuff up. The introduction of the Vision and him dealing with the ramifications of his origin, the personal conflict of the Black Panther, and of course Cap adapting to the modern world. All good stuff.

Worst Group: X-Men. This one is just far too obvious. The characters as a whole are entirely bland and uninteresting. Iceman and Angel are both pretty obnoxious, and Cyclops whole "I can't express any feeling because the powers I seem to have perfectly under control might one day be a danger" thing is utterly stupid. And Xavier is a dick.

Best Romantic Subplot: None of these were particularly good IMO, but Thor/Blake/Jane was the one I liked the most. Sure it was predictable, but Jane dreaming of polishing Thor's hammer pretty much makes up for everything else.

Worst Romantic Subplot: Matt/Mike/Foggy/Karen. Matt considered proposing to Karen as Mike, 'nuff said.

Best Villain: Doom is the only one who I though had much in the way of development and character. Plus the dude's just awesome. Special runner up prize for that one guy who impersonated the Thing in what is easily one of my favorite issues in the order yet.

Worst Villain: Mekano! AARGH! Lame villain with lame abilities and the single stupidest motivation for a villain yet. I can't hate this guy enough.

Since you mentioned supporting characters, I thought Mary Jane and Hogan are great so far.

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1-332 with a fair amount of knowledge of what is coming due to having read the majority of them over the years.

Best Character: Iron Man - I hate the woe is me subplot, due to his heart, that Stan Lee loved so much, but otherwise I really like the character.
Best Villain: DOOM!
Best Group: At this point in the order I have to go with the FF.
Worst Character: I had to think hard about this one but Hank Pym wins, though Daredevil was close and I find myself dreading Spider-man because I get tired of him feeling sorry for himself.
Worst Villain: The Matador - only three appearances in the first 30 years of Marvel. Even the writers don't like him. Daredevil got some really lame villains, but this guy is the worst.
Worst Group: The Avengers Mk II. Watching Quicksilver and Hawkeye trying to take command from Captain America is just painful. Thankfully I know things get better later.
Best Supporting Character: Volstagg always makes me laugh. Honorable mention to Happy Hogan for being smart enough to figure out Iron Man's identity.