I never cared much for raw graphic horsepower, but some of the games that left me in awe when I saw them (whether because they had the "wow, this thing looks like watching a cartoon!" or because I really -- I mean REALLY -- loved the art direction) are, in no particular order:
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Broken Sword: Shadow of The Templars (I had played loads of point and click adventures before, but this one felt like playing through your own Disney/Dreamworks animated movie, at the time);
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The Legend of Zelda: A Link to the Past (I know it's nothing special by today's standards, but back then I felt like playing an actual cartoon in video game form, at least for me);
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The Legend of Zelda: Wind Waker (say what you will, cel-shaded graphics rock, and they age way better than photo-realistic ones, the original GCN version still looks absolutely gorgeous and charming);
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Psychonauts (The Milkman Conspiracy. Black Velvetopia. Need I say more?);
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Stick It to The Man! (awesome art design!);
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Guacamelee! (see Stick It to The Man!);
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Ether One (it's beautiful. Seriously. As soon as I get some money, it's going to be the first game on my GOG wishlist I'm buying!);
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Shadow of the Colossus (it's amazing what they did just relying on atmosphere and using minimalistic design. One of the best looking games ever, in my humble opinion);
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Silent Hill 3 (I played it on the PC and, my god!, it looked amazing! It's not my favorite one in the series, that honor goes to the second title, but 3 was the one that impressed me the most, visually. I think I had to get a new GPU in order to play it properly, too);
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Legacy of Kain: Defiance (I remember the game box quoting something along the lines of "the best looking Kain to date". And it was. Being a fan of the LoK series since the beginning, having fallen in love with Raziel and his storyline in Soul Reaver, after a "meh, just a cool vampire story" with Silicon Knights' Blood Omen, and having played every single game in the series along the years, seeing Raziel and Kain in such a level of detail and gameplay fluidity almost brought tears to my fanboy eyes);