I like it because it's a very immediate device no loadings, it can be closed to save battery when you have to pause the game, even for long times...What I mean is that it's the ideal console to play quick games during breaks, it doesn't always require the same dedication and amount time to get involved into the experience as on home consoles.
Than compared to the PSP I don't know. Form what I've seen and tried, it doesn't tempt as much as the DS because It doesn't seem to me quite as handy: it is bigger, it has loading times, the battery don't last very long, games on UMDs are generally more expansive and also not as portable as DS cards.
The PSPgo seems to solve all this problems but at the moment it's just too expansive and considering that the 3DS may be coming quite soon (maybe also the PSP2), it dosen't tempt me much either.
Considering games at last it seems to me that, in terms of quantity there are more quality games on PSP than on DS, but still many of those are portable verisions of PS2/PS3 games. That's not necessarily a bad thing, but choosing only one protable I prefer the DS which offers different games I couldn't play on home consoles.
With that said I don't think that the DS is immune from defects, the lack of an anlog stick can be quite annoying sometimes (Mario64 DS for example), this plus it's lower rendering power (compared to the PSP) doesn't make it the ideal platform for open-space 3D games.