The bosses in Resident Evil games tend to be the size of sky scrapers and adorned with tentacles, so I'll go with the final boss in Darkside Chronicles.
I would say most of the colossi in Shadow of the Colossus, but I remember most of the bosses in Bayonetta being pretty damn big as well. Especially the final one.
Probably the Titan from the 1st PSP GoW game, i didn't really kill him, but the poor guy was left there holding olympus or earth or whatever it was for the rest of his life or until another sequel that i havent played.
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