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One game I was ridiculously impressed with graphically was Dragonsphere which I discovered simply by signing up for GOG!
The animation is so fluid, I couldn't believe it.

Someone has mentioned Simon The Sorcerer 4 & 5 and a lot of people have mentioned the Lucasarts adventures, but I would say that Simon The Sorcerer 1 & 2 beats ALL of them.

Especially Simon 1.

I'd never seen an adventure game that pays so much close detail to it's environments as the first Simon and I have to say that it is probably my favourite point-and-click adventure game and that is mostly due to the lovingly crafted pixel-art in the backgrounds and foregrounds of it's world!
not PC games but nonetheless....

The Metal Slug series

Those games have an absolutely ASTOUNDING Attention to detail, everything is so sharp and fluid in them, I can only imagine the amount of work developers spent animating those pixels