"Prime Time of Your Life/The Brainwasher/Rollin' n Scratchin'/Alive" from Alive 2007. It comes off really unsettling until "Alive" kicks in.
The first minute and a half of, "Touch" is...very very unnerving.
The last few lines of it however, are rather tearjerking.
"Contact", especially the second half, is extremely unsettling, sounding very distorted and eerie.
"Within" has very eerie lyrics, compared with the creepy as hell robot voice.
In The Collaborates: Pharrell Williams, Pharrell talks about how the beat of the music mimics the rhythm of a human heart beat, with a black-and-white animation of a heart plays in the background, then it fades to a strange machine, an artificial heart, showing how they are robots. While this does not seem very creepy on its own, it is once you realize where those clips are from...