- Pretty much any PlayStation 2 re-release:
- Metal Gear Solid HD Collection
- The Sly Collection
- Ratchet & Clank Trilogy (Digital only in USA - UK had a physical release)
- Jak and Daxter Collection (Look around before purchasing the game - I've heard various complaints about the framerate)
- God of War
- Final Fantasy X/X-2
These were all really great titles you should try had you not got to experience them on the PS2 or any other platform. It's also great to have them on a handheld.
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Sonic All-Stars Racing Transformed. A port of the console/PC release that pretty much has no content cut. All they did was downgrade the visuals, and it's an amazingly fun kart racer. Think of Mario Kart on steroids and with a more balanced characters/item roaster. Even on the Vita a lot of the tracks are breath-taking to race around at breakneck speeds, and all three "vehicle types" offer for a lot of nice variety. Having this game on the go is incredible.
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LittleBigPlanet Vita. The Little Big Planet I really loved. A very charming platformer with a huge focus on creativity.
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Persona 4 Golden. A port of a PS2 title but it adds a lot of content that makes the game worth it. I haven't played it but there's a lot of content here and a lot of people point to it as the best title for the Vita. Give it a shot if you think you might like JRPGs.
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Gravity Rush.
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Rayman Origins and Legends. Beautiful 2D platformers that are as tough as nails but the art style and level design more than makes up for it. The Vita ports are pretty good. The Vita port of Legends cut out some levels apparently, but a patch can be downloaded from PSN now that restores them I think.
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Wipeout 2048. Cool futuristic racer. Not sure if it's as good as All-Stars Racing Transformed but it's definitely worth looking at.
Digital Only Titles:
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TxK. A really cool "modern" version of Tempest 2000 with trippy visuals and a soundtrack. Can be pretty addicting.
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Super Meat Boy. Great port of a great but tough as nails 2D platformer. Even with the changed soundtrack it's buttery smooth and it feels pretty great on the Vita with it's "pick up and play" gameplay yet insanely challenging levels.
There are probably some other great indie ports, but I haven't tried them yet. I'd recommend waiting on these though if you're still on 3.60 as a firmware spoofer for the Vita might be possible now.