Three-dimensional　heterogeneously　nanostructured　thin-film　electrodes　were　fabricated　by　using　Ta2O5　nanotubes　as　a　framework　to　support　carbon-onion-coated　Fe2O3　nanoparticles　along　the　surface　of　the　nanotubes.　Carbon　onion　layers　function　as　microelectrodes　to　separate　the　two　different　metal　oxides　and　form　a　nanoscale　3-D　sandwich　structure.　In　this　way,　space-charge　layers　were　formed　at　the　phase　boundaries,　and　it　provides　additional　energy　storage　by　charge　separation.　These　3-D　nanostructured　thin　films　deliver　both　excellent　U-ion　battery　properties　(stabilized　at　800　mAh　cm(-3))　and　supercapacitor　(up　to　18.2　mF　cm(-2))　performance　owing　to　the　synergistic　effects　of　the　heterogeneous　structure.　Thus,　Li-ion　batteries　and　supercapacitors　are　successfully　assembled　into　the　same　electrode,　which　is　promising　for　next　generation　hybrid　energy　storage　and　delivery　devices.