I will always be impressed with how ripped Tobey got for the role. It was absolutely incredible. Until that famous scene in SM1, I didn't know abs could actually look like that :S
I didn't like his Peter Parker. I found him to be quite dull - he had some good lines though, but I never felt any weight behind them - "sometimes we have to be steady, and give up the thing we want the most."
Garfield adds a depth to his role that Tobey didn't. But I'll never forget Tobey - he was the first, just not the best.