With me, the thing that makes the original two so magical is the expert casting of extras.
Their reactions to Spidey's derring-do's made the whole CG enhanced spectacles work.
My favorites are:
Spider-Man (2002): The scene on the bridge when the Goblin is obstructed from killing Spidey (and MJ,) by a mob of folks with bricks. When one shouted that he was picking on a bunch of kids and finished with "You mess with one of us, you mess with all of us!" was the most memorable scene in the whole affair. So much emotion, you don't have to be from NY to get choked up with pride. Spider-Man becomes a symbol to the city of hope, much like the NY jumper did in "14 Hours."
Spider-Man 2 (2004): Yes, the train scene was masterful, with a well cast batch of passengers, who practically all get a line or two. But, it was that scene where he's delivering a pizza by moped and stops a car careening into a crowd with a web. In fact a pretty lass, says "a web," in the most believable way of wonder and relief. Her "Go Spidey, go!" was our collected breaths of the pay-off for the crowd who were miraculously saved.
There's so many more scenes too, the two little boys and the guy in the elevator in part 2, to name at least a couple more.
All you see in the 3rd and the Garfield ones are just reaction shots in crowds (very similar to Ashley Johnson's role in The Avengers, before her 5-second interview.) They needed those talented actors to help sell the scene they were in, with little gestures and dialogue.