AbstractHerein, a novel combination with a focused morphology is designed after synthesizing CrVO4 (CV) nanoparticles and poly‐pyrrole nanotubes (PNT or P) to prepare the interlocks of the composites of PNT and CrVO4 as 1PCV1, 1PCV2, 2PCV1, and 2PCV2 to study the supercapacitor application. Structural and spectral characterizations are perpetuated to confirm the synthesis of the samples. Results furnishing best energy storage are obtained for the intercalated composite 2PCV1 examined for three‐probe and two‐probe set‐up. The excel values for specific capacitance (Cs) for 2PCV1 concerning the Cyclic voltammetry (CV) cycle and Galvanostatic Charge Discharge (GCD) curve are 1745.60 F g−1 at 10 mV s−1 rate and 1545.62 F g−1 at 0.625 A g−1 current density studied along with interface controlled and transport‐controlled Cs with a contribution of 55.13% interface part and 44.87% transport part at 5 mV s−1 scan rate. Electrochemical Impedance Spectroscopy (EIS) study has provided 0.86 n‐factor with solution resistance Rs of 1.48 Ω, and a charge transfer resistance of 0.166 Ω. The respective specific power and specific energy values obtained through the two‐probe set‐up are also interestingly high 416.68 W kg−1 and 45.14 Wh kg−1 at 0.83 A g−1 current density. Also, the retention % in Cs values is studied by running 5000 continuous voltammetric cycles with 96.23% retention in supercapacitor device.
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