Polymeric polypyrrole-like (PPy-like) nanocrystallines were fast synthesized through oriented plasma polymerization at atmospheric pressure and room temperature. The effects of discharge power on the nanocrystalline morphology were investigated. Larger power tends to produce longer nanocrystallines. 3 mm long nanowires were produced at the largest power in our experiment. TEM image and the sharp electronic diffraction spots in SAD suggest that the nanoparticles have a single crystal phase. The chemical structure of the nanocrystalline has been studied through FTIR, EDX etc. This novel polymerization method could have great applications in fabricating functional polymeric nanocrystallines.