Demand increasing for next generation portable and miniaturized electronics has aroused much interest to explore microscale and lightweight energy storage devices. Herein, we demonstrate successful development of flexible wire-shaped microsupercapacitors (micro-SCs) based on novel CoNi 2 S 4 /E-NZP film@Cu wire electrode. The etched Ni−Zn−P (E-NZP) film was synthesized by directly deposition of NZP film on Cu wire, followed by a chemical etching process. Alkaline etching treatment provides a micro-and mesoporous structure with high surface area and facilitates the penetration of electrolyte ions into the electrode matrix. Then, CoNi 2 S 4 nanosheets as electroactive material are electrochemically grown onto the E-NZP film@CW electrode under a constant potential. The synergistic effects contributed by various components inside the CoNi 2 S 4 /E-NZP@CW electrode deliver superior performances with a high specific capacitance of 1.12 F cm −1 , 8.9 F cm −2 , and 889.68 F cm −3 at 4 mA cm −2 , outstanding rate capability (0.66 F cm −1 , 5.3 F cm −2 , and 529.02 F cm −3 at 80 mA cm −2 ) and long-term cycling stability (93.4% capacitance retention after 7000 cycles). Moreover, a flexible solid-state asymmetric micro-SC is fabricated using CoNi 2 S 4 /E-NZP film @CW as the positive electrode and rGO-coated carbon fiber (rGO/CF) as the negative electrode. The fabricated device exhibits high length, areal and volumetric capacitances of C L : 40 mF cm −1 , C A : 0.241 F cm −2 and C V : 18.54 F cm −3 , good mechanical stability with a maximum energy (E L , 18 μW h cm −1 ; E A , 108.4 μW h cm −2 ; and E V , 8.34 mW h cm −3 ), and power densities (P L , 1454 μW cm −1 ; P A , 9280 μW cm −2 ; and P V , 716.9 mW cm −3 ). This work provides a new and facile approach to develop high-performance wire-shaped electrodes as a new generation in energy storage applications.