This paper presents a new concept for making battery electrodes that can simultaneously control macro-/micro-structures and help address current energy storage technology gaps and future energy storage requirements. Modern batteries are fabricated in the form of laminated structures that are composed of randomly mixed constituent materials. This randomness in conventional methods can provide a possibility of developing new breakthrough processing techniques to build well-organized structures that can improve battery performance. In the proposed processing, an electric field (EF) controls the microstructures of manganese-based electrodes, while additive manufacturing controls macro-3D structures and the integration of both scales. The synergistic control of micro-/macro-structures is a novel concept in energy material processing that has considerable potential for providing unprecedented control of electrode structures, thereby enhancing performance. Electrochemical tests have shown that these new electrodes exhibit superior performance in their specific capacity, areal capacity, and life cycle.