The song was first "heard" (short version) on the collaboration video entitled CMPV R/L 2; a 27-minute video, a collection of short PVs by various illustrators in celebration of the Kagamines' birthday on 2011.
The same day it was uploaded; a short version was uploaded to Nico Nico Douga as Patirchev's entry on the game Project Diva Arcade. It was also a part of the entry for the compilation "V Love 25 ~Cantabile".
Unreal Communication tells a story of Rin and Len; who were apparently robbers / thugs (as mentioned, they're Bonnie and Clyde; a pair of married murderers and thieves on the 1900s). The two fell in love though for an odd reason they find it hard to "communicate".