Here, we report Si pillar and well arrays as tailored electrode materials for advanced Li ion storage devices. The well-ordered and periodic morphologies were formed on a Si electrode thin film via laser interference lithography followed by a dry etch process. Two different patterns of negatively or positively carved Si electrodes exhibited highly improved cycle performance as a consequence of the enlarged surface area and the nanoscale pattern effects. The Si well arrays showed the highest energy density, rate capability, and cycling retention among the prepared Si electrodes. This tailored electrode platform demonstrates that these design principles could be applied to future developments in Si electrodes.