Maybe you are not missing anything, you just don't like him, and he can't convince you for some reason. It happens.
As for me, I only discovered him in Avengers however I had been aware of his existence before that. He could convey Banner's restrained anger pretty convincingly and he made me pay attention to his every movement and expression. And it was before I became a fan, so I wasn't biased yet. He could create an atmosphere around Banner that made him look really dangerous and loveable (and a little bit piteous) at the same time.
I think he has a very expressive face and suggestive eyes. A lot of people don't like his voice and the way he talks, and this fact can prevent them from relating to his characters. But I think it's unique and nothing's wrong with it.
Some examples of his good acting (of course it's just my opinion...if you are really interested in it):
You Can Count On Me:
Undeniably one of his best performances. He looks really lost and vulnerable, someone who you want to save or at least hug, but who can also make you mad. From his first appearance he can make the viewer feel what Laura Linney's character feels about him, it's like he is your brother or friend who you are really worried about. There is always something painful behind his smile and he uses his voice very well in this movie. It's sweet and fragile.
What Doesn't Kill You:
He totally disappeared in Brian's character, even the way he walks is really different from what he did in his other movies. All of his moves contain an interesting mix of toughness, fear and guilt. The looks he gives when he is trying to be a good father and husband (and constantly fails in that) are very real. I like his accent in this, though I'm not English so I can't tell if it's accurate.
We Don't Live Here Anymore:
There is one scene near the end (it can be a spoiler) where his character decides he doesn't really want to leave his wife (Laura Dern) and asks her to unpack his bags. He is close to crying and in his eyes you can see all the bad choices he had made, the things he had messed up in his life and the recognition that a new relationship wouldn't make anything better. He is good in the other scenes too but this one is the most heartbreaking.
In The Cut:
The movie is not too good (though has some nice moments), but Malloy's character is exciting. He is very confident and manly but there is a little sadness about him too. The chemistry with Meg Ryan is good, the first time he puts his arms around her is hot, in a very unique way. I also like his accent here and his "macho-cop" talking. He is very attractive despite the funny mustache and "far from perfect" haircut.
The Kids Are All Right:
It's just really natural, like he was not acting at all, just being there and have fun. But it's obviously not true because the character is very different from him. (Apparently I don't know him, but he is married with three children, and is far from being a hopeless bachelor who just longs for a family. And I assume he has never slept with a lesbian woman's wife. Though I can't be sure about the second one. :D )
The Normal Heart:
He could play very convincingly that he was gay and in love with another man. There is a debate on the movie's board about his "yelling", if that was passionate enough or not. For me the key word was not passion in those scenes, but frustration, despair and pointlessness (since nobody really listened to him). That was quite beliveable. I also felt it was sometimes a little bit tiresome but I think it was part of that character.
Well, these are my reasons...Sorry for writing so much, but you asked for them.:)
To answer your last questions... Yes, I honestly think he is really good at what he does. My political views are mixed, I consider myself somewhere between liberal and conservative. I had started to like Ruffalo before I knew anything about his views and activism. I have to admit that I don't know anything about fracking and really little about global warming and environmental stuff. I respect people who stand up for causes they believe in, but it has nothing to do with acting abilities, so I don't build my opinion about an actor's work upon this.
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