We have proposed a novel plasma processing, i.e., radical-controlled processing using radical injection technique, and demonstrated the formation of carbon nanowalls (CNWs) using fluorocarbon plasma-enhanced chemical vapor deposition assisted by hydrogen atom injection. CNWs can be described as the two-dimensional graphite nanostructures with edges, which are composed of the stacks of plane graphene sheets standing almost vertically on the substrate, forming wall structure with high aspect ratio. Growth mechanism of CNWs was discussed on the basis of density measurements of important radicals in the plasma. Moreover, CNWs were formed by using the multi-beams of fluorocarbon radicals, hydrogen atoms and ions, and the effect of ion bombardment on the nucleation of CNWs was investigated.