Soft lithography using polydimethylsilicate molds is shown to be a novel promising method to prepare three-dimensional (3D) micro Li-ion electrodes, demonstrated by the synthesis of nanometer TiO2 anatase in the molds via a TiO2 sol. With this approach the 3D electrode morphology can be controlled to a large degree, which allows for the optimization of ionic and electronic wiring. The resulting 3D microshaped nano-TiO2 electrodes, with no conducting or other additives, show very high rate performance in combination with high electrode densities (energy densities) and long cycle life. These results demonstrate the potential application of soft lithography techniques for high-performance electrode preparation which, in addition to providing a large degree of control over the 3D electrode design, is relatively cheap and easy to scale up.