Aluminum nitride (AlN) is a key material for microelectronic devices. Multilayered porous AlN materials are synthesized for the first time using 2D carbon nitride organic materials as a template. Moreover, unique morphology with multiscale pores and a large specific surface area is beneficial to its electrochemical energy storage. As an electrode material, porous AlN presents an excellent specific capacitance and good cycling performance (10,000 charge/discharge cycles). Also, the capacitance is positively enlarged after 6000 cycles. Furthermore, the fabricated AlN symmetric supercapacitors (SCs) using a neutral electrolyte also manifest a high energy and power density of 3.88 μW h cm −2 and 4.25 mW cm −2 at 10 mA cm −2 , respectively, and excellent cycle performance (98.14% retention after 10,000 cycles) and light up the light-emitting diode lamp. This research proposes AlN as an anode and cathode material for the SC device and also suggests the significant potential of AlN as important materials for the microelectronic devices.