Radiohead - Karma Police

For me, it just doesn't get much better then this song. It's structure is not in the form of a typical song. You don't go from verse to chorus to verse to chorus to outro. The tempo completely shifts for a short 2 verses. 'This is what you get when you mess with us' and then the song returns to the basic 4/4 time signature. Sometimes, simple is best. Just when the song feels familiar the melody starts to unravel the entire song ascends into an airy wisp 'For a minute there, I lost myself'.

An interesting note is the beginning of the song is in A Dorian. ;)