Electrophoretic deposition is presented as a handy and cost-effective technique to transfer nano-sized (powdered) electrode materials into thin-or thick-films for electrochemical energy storage applications. Electrophoretic deposition of Li4Ti5O12 nanoparticles is studied to prepare thick films as anodes for Li-ion microbatteries with MgCl2 additives-for the first time-as an efficient charging agent and a source of binder simultaneously. Electrochemical measurements in lithium test cells confirmed that the prepared thick-film Li4Ti5O12 electrode has good discharge (lithiation) capacities and cyclability, as well as good electronic and Li + transport properties. Indeed, electrophoretic deposition is demonstrated to be a suitable alternative to prepare self-supported micro-or nano-structured Li4Ti5O12 for Li-ion microbatteries.