A three-dimensionally ordered macroporous FeO/Al nanothermite membrane has been prepared with a polystyrene spheres template. The nanothermite, with an enhanced interfacial contact between fuel and oxidizer, outputs 2.83 kJ g of energy. This is significantly more than has been reported before. This approach, fully compatible with MEMS technology, provides an efficient way to produce micrometer thick three-dimensionally ordered nanostructured thermite films with overall spatial uniformity. These exciting achievements will greatly facilitate potential for the future development of applications of nanothermites.