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The best games for 3DS are generally considered to be Kid Icarus Uprising, Fire Emblem Awakening and Zelda Link between Worlds.

In my opinion, Kid Icarus and Fire Emblem are much more replayable the Zelda Link Between Worlds. The % of people who have over 100 or 200 hours in those 2 games is surely many times higher.
Kid Icarus has very polarizing controls, if you can manage the controls you will think the game is a masterpiece, but if you hate the controls you may not be able to finish it.
Link between worlds is also great, but you will probably beat it in 15 hours, so if you beat it twice, one in normal mode and one in hero mode (hard mode) that is about 30 hours.

Ocarina of Time is great, and is a must play if you never played Ocarina of time.

Super Mario 3D Land is a very good Mario game, although not a Masterpiece like mainline console Mario generally are.

Resident Evil Revelations is a good resident evil game (feels more like a resident evil game than 5 or 6), the 3D helps to make it more spooky, and it is one of the games that pushed the 3DS the most.

New Super Mario Bros 2 is good, not great.
According to most people who played Bravely Default, the games first half is much better than the second half

The rest of the games aren't that good

Metal Gear Solid 3 snake easter is not a very good port, play the hd version on PS3 VITA or Xbox360.