This work describes a new orientation method for semicrystalline poly(3-hexylthiophene) (P3HT) thin films, coupling nanorubbing and subsequent crystallization. Using the stylus of an atomic force microscope, we align the polymer chains on P3HT surfaces with a spatial and geometrical control of the oriented domains (nanorubbing). These chain-aligned structures can be made permanent thanks to the crystallization process, which propagates the orientation obtained at the surface to the bulk.