Definately MarioKart. Also, Kirby: Squeek Squad & Yoshi's Island DS are really fun for anyone of any age, and if she likes New Super Mario Brothers, she should really like them. (I'll admit, the game play is a tad more intensive with those, but she shouldn't have too many problems.)
Final Fantasy: Chocobo Tales is very cute, has great game play, and puts some really nice Final Fantasy twists on some old fairy tales. If you'd like to get her into an RPG without throwing her straight into something heavy like Final Fantasy III, Chocobo Tales could be a great way to go. Also, Poke'mon Diamond/Pearl is a very light RPG, but with some absolutely awesome game play, and a LOT of continued playability. I'm not quite sure how well a 5 year old would handle Poke'mon, but my brother was about 7 when he started in on them, so it shouldn't be too far of a stretch :)
And this suggestion is, well...subjective. I was a baby-gamer on the NES at two years old, and one of my favorite games was/is Tetris. Personally, I think it's simple enough for a younger gamer to understand, and it helps develop thinking skills. Tetris DS has a lot of improvements over the original, and it's got lots of fun new things to try, so I would seriously consider getting that to throw in a bit of higher-thinking skills with her fun :)
Personally, at 5, I would say a good chunk of DS games would be fun for her, especially since there is very little hack/slash, extreme violence on the DS.
And can I just note: you're an absolutely killer big cousin :)
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