Two types of periodic surfaces were fabricated by utilizing two-dimensionally ordered arrays, in one case as a template and in another as a mask. In the first case, a bulb-like microstructured surface was formed, and, in the second, a cylinder-like microstructure. The Raman spectra of these films indicate that they consist mostly of diamond and therefore have a high refractive index as well as other well-known properties of diamond, making them attractive for photonic, electronic, and electrochemical applications.