We report a simple method to achieve efficient nanostructured organic photovoltaics via patterning copper iodide (CuI) nanocrystals on indium tin oxide by glancing angle deposition. The strong interfacial interaction between zinc phthalocyanine (ZnPc) and CuI leads to the formation of nanopillar arrays with lying-down molecular order, which greatly improve light absorption and surface roughness for exciton dissociation. Optimized ZnPc/C(60) bilayer cell has a power conversion efficiency of 4.0 ± 0.1%, which is about 3-fold larger than that of conventional planar cell.