I don't know about Spotify, but last.fm pads it's number of tracks with a lot of stuff that's no name bands that are really crappy and not available elsewhere. I know this because when I first got it and it hadn't tracked any of my listening habits, it only played the crappy stuff. Now that it's scrobbled 70,000 plays, it's a lot more accurate, however, it doesn't have a lot of the bands Iisten to, and Pandora does.
I also like how I can set up a station in Pandora based on a group or genre. It's a great way to explore new music. I recently discovered the band Earth. I never heard anything quite like it before and set up a station based on the band and everything it played was new to me and I liked it. I've done the same with some genres that I'm not that familiar with. I don't see how to do this in the last.fm app on my iPhone. Is that something you have to set up first in the desktop app or web app?
The one problem I do have with Pandora is that it can be incredibly repetitive, not only playing the same groups, but the same songs.
I have one question about Spotify premium. Can you search and download music to an iPhone, or does everything have to go though the desktop app. If I got Spotify, it would be to replace MOG. I use MOG only from my phone. I can't see Spotify's desktop app as something that would be useful for me. I'm usually nowhere near my computer when I decide to download an album.