Electrode materials with unique nanoarchitecture, great conductivities, and desirable mechanical stabilities are essential for developing nearly all energy storage devices (ESDs). Herein, a low‐cost route for the fabrication of double‐layer CuCo2S4@Ni−Mo−S (CCS@NMS) nanosheet arrays as an advanced binder‐free positive electrode for supercapattery is presented. The CCS@NMS porous nanoarchitecture has the advantages of good ion diffusion and excellent electronic transport. Accordingly, when employed as battery‐type electrode in supercapattery device, the CCS@NMS electrode reflects amazing capacity (Cs) of 446.3 mAh g−1 (3213.6 F g−1) at 1 A g−1 and 375.8 mAh g−1 (2705.85 F g−1) at 18 A g−1, and 98.2 % of the Cs was still maintained at 6 A g−1 after 5000 cycles, which are higher than that of CCS electrode. Most importantly, using the CCS@NMS electrode as the positive electrode and active carbon (AC) as the negative electrode, the device indicates notable Cs of 66.8 mAh g−1 (160.4 F g−1), the considerable specific energy of 50.125 Wh kg−1 at a specific power of 750.04 W kg−1 and outstanding robustness of 96.8 %.