“Two-for-one” strategy is an effective method to construct two kinds of materials from a single precursor owing to the simplicity of fabricating procedure and reduction of manufacturing cost. However, such a strategy has seldom been utilized to produce both battery-type and capacitive electrodes of a hybrid supercapacitor (HSC) device. Here, we adopt the “two-for-one” strategy to fabricate three-dimensional (3D) porous iron-doped (Fe-doped) Co3O4 and nitrogen-doped (N-doped) carbon via a single bimetallic metal–organic framework, FeCo-ZIF-67. Fe-doped amounts and carbonization temperature are used to adjust their individual electrochemical behaviors. The optimal 3D porous Fe-doped Co3O4 and N-doped carbon possess a high capacitance of 767.9 and 277C g−1 at 1 A g−1, respectively. Charge storage mechanism of Fe-doped Co3O4 is further investigated via analysis of capacitive and diffusion-controlled contribution. A Fe-doped Co3O4//N-doped carbon HSC device achieves desirable specific energy (37 Wh kg−1) and power (750 Wkg−1), and satisfied cycling stability (90% retention after 4000 cycles). A light-emitting diode (LED) is successfully light by the HSC device, suggesting its potential application in the field of green energy conversion and storage devices.