A new concept for making battery electrodes to simultaneously control macro-/micro-structures of electrodes is developed to address present energy storage technology gaps and meet future energy storage requirements. This new fabrication process fully utilizes the benefits of additive manufacturing, which provides a pathway for inexpensive and flexible production of specialized products. Furthermore, the process allows a simultaneous control of the microstructure and macrostructure of electrodes which cannot be achieved via conventional manufacturing techniques. Modern batteries are fabricated in a form of laminated structures that are composed of randomly mixed constituent materials. Due to this randomness, there is an ample room in the conventional method to enhance performance by developing viable processing techniques to construct well-organized structures. 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 and enhancing performance. Electrochemical tests show that the new electrodes exhibit superior performance in their specific capacity, areal capacity, and life cycle. It is concluded that the macro-micro-controlled structure showed 21%, 16%, and 7% more areal capacity than a structure with no control, a macro-controlled structure, and a micro-controlled structure, respectively The proposed control of 3D structures, with a well-organized distribution of energy materials, demonstrated more superior properties and advantages than structures with randomly distributed materials.