active material used in lithium batteries. Due to the many advantages on thin-film electrodes over powder-based electrodes, including their high purity, perfect stoichiometry, and freedom from the additives and binders used in the latter, preparing thin film electrodes via versatile deposition technologies undoubtedly has proven the most facile effective way to gain insights into the needed intrinsic properties of lithium-storage materials. In addition, the knowledge obtained from the preferred orientation and anion doping of such thin films by reactive RF sputtering, as well as from patterning thin-film electrodes, could well enrich our understanding of lithium electrochemistry that will be invaluable for lithium storage.