Virtue's Last Reward. Do it.
Play 999 for DS first if you haven't. These are seriously among the best games I have ever played.
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Big Kingdom Hearts fan here so if you are into/interested in them I would recommend Dream Drop Distance.
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Haven't ever played the series before, but the game looks good. Plus it appears to incorporate Mickey Donald Goofy: The Three Musketeers, a movie which I remember vividly from childhood.
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Ocarina of Time 3D is the same game it has always been. If you want to replay it, or never played it before, I'd reccomend you buy it.
From what I have played, Shinobi was quite fun. If you liked the other games in the series, grab it, it is also relatively cheap, even for a new copy (costs about 10 euros new, where I live).
Pokemon X/Y are obvious reccomendations.
Virtue's Last Reward is quite good, as well.
Then there's Project X Zone, which I enjoyed a lot.
For eShop titles, Mighty Switch force and Pushmo/Crashmo were quite good.
Oh, and of course don't forget Monster Hunter 3 Ultimate, Kid Icarus: Uprising, Fire Emblem Awakening and Resident Evil: "Revelaitons" (yes, I have one of those copies :D).
All of these are worth your money. There are many more games worth having, for the 3DS, but these are the best ones out there. In my opinion, of course. :)
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DS
Radiant Historia
Dragon Quest IV: Chapters of the Chosen
Dragon Quest V: Hand of the Heavenly Bride
Dragon Quest VI: Realms of Revelation
Dragon Quest IX: Sentinels of the Starry Skies
Shin Megami Tensei: Strange Journey
Mega Man Zero Collection
Mega Man ZX
Mega Man ZX Advent
Ghost Trick: Phantom Detective
Phoenix Wright: Ace Attorney
Phoenix Wright: Ace Attorney: Justice For All
Phoenix Wright: Ace Attorney: Trials and Tribulations
Apollo Justice: Ace Attorney
Nine Hours, Nine Persons, Nine Doors
Kirby Super Star Ultra
Kirby Canvas Curse
3DS
Etrian Odyssey IV: Legends of the Titan
Shin Megami Tensei: Devil Summoner - Soul Hackers
Shin Megami Tensei IV
Rune Factory 4
Pushmo
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Monster Hunter 3 Ultimate, it lasts hundreds of hours and provides lots of fun, bonus points if you have friends with 3DS with Monster Hunter 3 Ultimate, or a WiiU with MH3U.
I have yet to play multiplayer, since I don't know anyone with the game but I just reached 200 hours of gameplay, I bought it 6 days after it came out and I still enjoy the game.
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I got my 3DS (on craigslist) and a friend let me borrow Fire Emblem. Holy crap that game is awesome. Although I'm afraid I'm going to regret doing classic mode soon.
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Back again to annoy you with one more 3DS question.
For some reference, my favorite DS games were Chrono Trigger, New Super Mario Bros., the Prof Layton series, Mario Kart, Super Mario 64, Animal Crossing: Wild World, Sonic Classic Collection.
Some non-DS favorites are the Portal games, other Zeldas, Minecraft, Civ, and To the Moon.
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