Radical-polymerized chemical vapor deposition, a new bottom-up method, was developed to produce graphene nanoribbons (GNRs) efficiently, despite the use of extremely low vacuum. Using this technique, a systematic synthesis of a multilayered high-density array of width-controlled sub-1 nm GNRs on a metal surface, with width-dependent band gap, is made possible. GNR films transferred onto insulating substrates behave as an excellent photoconductor.