Three-dimensional ordered macroporous (3DOM) Al/NiFe2O4 nanothermite has been obtained by colloidal crystal templating method combined with magnetron sputtering processing. Owing to the superior material properties and unique 3DOM structural characteristics of composite metal oxides, the heat output of the Al/NiFe2O4 nanothermite is up to 2921.7 J g− 1, which is more than the values of Al/NiO and Al/Fe2O3 nanothermites in literature. More importantly, by comparison to the other two nanothermites, the onset temperature of 298.2 °C from Al/NiFe2O4 is remarkably low, which means it can be ignited more easily. Laser ignition experiment indicate that the synthesized Al/NiFe2O4 nanothermite can be easily ignited by laser. In addition, the preparation process is highly compatible with the MEMS technology. These exciting achievements have great potential to expand the scope of nanothermite applications.