Sly Cooper Triilogy

Before Infamous, Sucker Punch's trilogy of stealth-platforming games featuring cel-shaded graphics were some of the best family-friendly titles on the PS2. Because cel-shaded graphics tend to age more gracefully, they'd probably look a lot better on the PS3 than you'd expect.
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Final Fantasy X/XII (and XI?)

Final Fantasy XIII (and yes, XIV) keep teasing us with unending videos and trailers, but in the meantime there's no better time to revisit the two critically-acclaimed Final Fantasy chapters released on the PS2, both of which featured tons of cinematics begging for HD re-release. And, yes, perhaps for fun XI could be thrown in as well.
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Ratchet & Clank Collection

The PS3 games have been a revelation, but there are still three great games in the Ratchet & Clank series that could do with a bundle-pack re-release on Blu-ray--perhaps even with bonus content that could be loaded into the newer games.
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Metal Gear Solid 2 and 3

When Guns of the Patriots came out in 2008, we were among the many to pop out our old MGS games to replay the convoluted storyline one more time. And with the number of lengthy cut-scenes, they're almost better seen than played. But 4:3 letterboxing just won't cut it. Kojima, rescue us.
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Grand Theft Auto III/Liberty City/San Andreas

Grand Theft Auto 4 may have Niko Bellic and a photoreal NYC, but it still can't hold a candle to the world and scope of San Andreas. The 80's and 90's-themed PS2 GTA games were more cartoonish at times, more brutal at others, and well worth a serious revisit by Rockstar. And while we're at it, why not throw in Liberty City Stories and Vice City Stories as bonuses?
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Frequency/Amplitude

Before Rock Band, before Guitar Hero, Harmonix defined rhythm-music gaming with their cult-hit series of arcade games on the PS2. With a graphic look that hovered somewhere between Rez and Wipeout, their clubber-scifi aesthetic would be a refreshing break from Beatles overload.
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Ico/Shadow of the Colossus

Call this one the Team Ico Collection. With The Last Guardian coming to the PS3 sometime next year, we can look back to their incredible duo of PS2 titles in the meantime to hold us over. Both Ico and Shadow were artful, groundbreaking, and utterly classic games that defied easy explanation. They still look fantastic, but 16:9 HD upscaling would be a really nice touch.
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Jak and Daxter Trilogy

Naughty Dog's acclaimed Uncharted series on the PS3 is as entertaining as a box-office blockbuster, but their PS2 series of Jak and Daxter games had far more humor. Ending in 2004 with Jak 3, these are classic platformers that would be better off released together than separately.
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Kingdom Hearts/Kingdom Hearts 2

Disney characters plus Square Enix characters with giant hair and swords equal one of the strangest and yet successful mashups in all of video game history. Not only were the lengthy storylines well-constructed (and often impossible to comprehend), but the Disney-themed worlds were beautifully animated and designed. Until Kingdom Hearts 3 hits the PS3, the first two games would serve as a great introduction.
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