I mean, yes, Venom is clearly evil as he is only presented in a slightly sympathetic light when he is like "It's Brock, sir. Edward Brock Jr. I come before you today. Humbled and humiliated...". However, otherwise, he's just plain bad and even says "I like being bad. It makes me happy."
Norman/Green Goblin, is pretty selfish, but does seem to care for Harry somewhat, and does seem to keep having bad luck as at first, it seems the Goblin stuff is happening by mistake though it seems he knows more and more what's going on.
Also, one wonders how true it was when he said "I wanted to stop it, but I couldn't stop it.".
Also, his very last lines show that he at least cares for Harry, who looks up to his dad, er, somewhat, and doesn't want Harry to know what he's become.
As for Doc Ock, he seems to be more antihero than villain. He spent his life's work on his machine, he let his ego get in the way, his wife died and he got four new arms stuck to him. He wanted to still help the world but knew Harry wouldn't fund him anymore so he turned to crime and kidnapping (near the end). However, his last act was to save the others (Peter was going to try and stop the machine, but he said he'd do it.) (The Lizard from the Amazing Spiderman also seems to be more antihero as he at first wants to help the world and is being screwed over by Oscorop.)
Then there's Flint Marko. His daughter is dying and he is robbing, not just to get rich, but because she needs a lot of money to do some fancy operation or something. He kills Ben Parker when his partner grabs his shoulder, accidentally causing the gun to go off and, based on the conversation near the end of the movie, is regretful about that. He also seems to be doing this only for Penny, though I think him going after Spidey in the final fight may have had something to do with Spidey trying to axe him first. Also, oddly enough, he seems to be the only villain from the trilogy who DIDN'T die.
Then there's Harry Osborne. He is good for most of the first movie At the very end, he wants to kill Spidey (and, given Spidey came back with his dad's body but never explained what happened, it's easy to sympathize with him.)
In the second movie, he's mad at Spidey the whole time and won't even thank him for saving his life. He even turns on Peter at one point, though clearly Harry was drunk, slapping him and saying that he won't let him get justice for his father because Spiderman is his bread and butter.
Admittedly that deal to trade the tritium for Spidey was a bit dark, though forced as he was gonna be dropped. Also, he couldn't kill Peter, even though he knows he's Spiderman when he finally unmasks him and even though Peter STILL didn't explain what happened.
However, Harry later gets a visit from his father (what the heck!) and ends up smashing a mirror and finding the Goblin's lair.
In the third movie, even though he now knows his father's dark secret, he's STILL mad at Peter. He tries to kill Peter, though, he's nice afterward, though mainly due to amnesia.
Later, though, he recalls everything again, and makes MJ break up with Peter. Later, he and Peter get in a fight. Near the end, he still refuses to help Peter (can see why after what happened to his face!!!). It takes Bernard, who, oddly enough, NEVER bothered to mention this important fact sooner, to get Harry to realize how his father really died.
After that, Harry is nice and even gives his life to save Peter. (I wouldn't consider Harry Osborne/ New Goblin a villain anyway, as villains don't give their lives to save heroes.)
And, of course, there is Spiderman himself who seems more anti-hero.
In the first movie, he lets the robber get away to get revenge (which results in his uncle getting killed).
In the second movie, he actually quits being Spider Man for a while.
In the third movie, he's really not such a hero. He is stuck on himself and would rather take a picture of a "Spidey the Mighty" banner than MJ and is so stuck on himself that she feels that she cannot confide in him that she got let go from the show.
Then he goes and tries to murder Flint Marko. Then, he goes and beats Harry up and redecorates his face. Then, he goes and humiliates Eddy Brock in front of everyone. Then, he goes after MJ and humiliates her and beats up some guards and punches MJ. (How did they let him back in later?!).
All in all, the villains in the Spiderman trilogy, and maybe Spidey himself, seem more like antiheroes.