An electrophoretic deposition (EPD) method has been developed for the first time to prepare thin-film LiFePO(4) cathodes. The effects of polymers and surface-active additives in the electrolytic bath, voltage and deposition protocol have been studied with the aim of obtaining highly adhesive, compact pristine LiFePO(4) and polymer-LiFePO(4) composite films to be utilized in planar and three-dimensional microbatteries. The samples were investigated by scanning electron microscopy (SEM), energy-dispersive X-ray spectroscopy (EDX). XPS and TOFSIMS. These methods confirmed the presence of a polymer binder and its homogeneous lateral distribution in the composite EPD-LiFePO(4) cathode. Li/LiFePO(4) semi-3D concentric microbatteries (3DCMB) on perforated silicon substrates showed a peak-pulse-power capability of 175 mW cm(-2) and stable electrochemical behavior for over 200 cycles at 100% DOD. Coating the LiFePO(4) with a thin layer of copper sulfide improved the cell performance even more. The 3D-LiFePO(4)-CuS-coated batteries are capable of delivering peak pulse power greater than 200 mW cm(-2) and an energy density of 6-10 mWh cm(-2) - adequate for the needs of microsystems. (C) 2011 Elsevier B.V. All rights reserved.