Probably Sticker Star. Played it for a solid 26-27 hours or so. Longer than OoT, and it's the only 3DS game I've bought with any real length, if you don't count 3D Land since it's so short, or MK 7, which is just multiplayer.
Of course, I'm going to GameStop today after work to pick up my M&L pre-order, so the Sticker Star record will soon be beaten on my 3DS for longest playtime.