Ds and 3ds libraries are unrivalled and are two of my favourite consoles ever. On my 3ds I have about 7 3ds cartridges, 9 downloaded retail games, 23 3ds eshop only games, 8 dsi eshop games and 9 vc game. Plus I have the 20 vc games from the ambassador program. And I can't count my many ds carts because I left them all in England.
I have a psp which I use a lot for emulators and a few psp games. Being a good machine for emulators boosts the systems value for me a lot and it has a good dpad which many of the native psp games don't take advantage of. It's great piece of hardware, but I would say that many of the best psp games aren't the kind of games I want to play on a handheld.
I carry my psp around in my bag because I'm scare that if I lose my 3ds I'll not be able to recover my digital downloads. Honestly, Nintendo is a let down there.
The Vita seems to have a more varied library than the psp, thanks to indies, and is appealing to me.
Both 3DS and DS have spent significant periods of time as my primary gaming devices.