Any very smooth metal surface is not going to be particularly receptive to a new coating without some kind of surface preparation (like sanding and ideally some primer) before the color coat. I recommend powdercoating for a durable finish with an industrial look. I got my single speed mountain bike frame sand blasted and powdercoated by a powdercoating outfit for about $70. If you pick a popular color they can put your frame in with the next job in that color. Based on how the frame looked after the sandblasting, I imaging that sandblasting would remove chrome as well.

I have a Santa Cruz Roadster fixed gear that I may have powdercoated as well. The factory finish is very nice, but an employee of my local bike shop put a very small chip in the paint on top tube. He was extremely sorry but refused to let me take a hammer to his frame. The current electrician's tape repair is not a permanent solution.

Good luck.