I've just been listening to a podcast of This American Life and I was wondering what the song was from the end of episode 218: "Act V" (at 56:11 of the 58:33-length podcast; originally aired on 9 August 2002; recently aired on 1 July 2011).
I searched around on the TAL website, but couldn't find a track listing. Then I remembered I could use Shazam on my iPad. Turns out it's "Desperado" by The Langley Schools Music Project on their album "Innocence & Despair".
Download episode
Skip to 56:59 to hear the song in context.
Grooveshark
At the time I wrote this post in July 2011, you could listen to the song on Grooveshark, but that site is now defunct. You can hear the story of Grooveshark on the StartUp podcast.