ME! On the 3DS side:
I'm still in love with Zelda OoT. I'll be starting the Master Quest, soon.
I'm having a blast taking down those spammers who use auto-block and instant moves in SSF4 (How the fuck can you block a sweep kick while standing up!?)
RE Mercenaries turned out to be a lot of fun, too.
On the DS side:
I went back and got Chrono Trigger for the DS and I'll probably go back and get a ton of great DS games that I just didn't want because I was so in love with the PSP (Zelda Spirit Tracks, TWEWY). I'm giving Advance Wars a second go, too. I'm planning to give New Super Mario Bros., Mario Kart, and Mario 64 some attention when I run out of new games to play but that hasn't happened yet.
DSi Ware/Virtual Console:
I got Plants vs Zombies and Uno (even though I own both of them on the 360). Pretty good time wasters. I wish Uno's online allowed for microphone/camera support, though. And I heard that Shantae Risky's Revenge was a good game-I had no idea how good! This game reminds me of the best days of the SNES. I love it!
And of course, I use Netflix when I'm online. It's cool to have a movie playing in the background. I'll start using the camera and putting music on my 3DS now that I have a decent 8GB SD card. I've barely used the AR Games, Pokedex, and Face Raiders since getting the console. I'll get around to having fun with them, eventually. It's just too much content! I even find myself walking around with my 3DS, even when I don't plan on playing it just so I can keep track of my steps and maybe meet someone with the Spot Pass.
Looking forward to my free ambassador games, too! And MGS3, Starfox, Kid Icarus, Super Mario, RE Revelations, and Mario Kart in the future, as well.