Abstract Rechargeable aqueous zinc‐ion batteries (ZIBs) have attracted extensive interest owing to their low cost and high safety. Herein, oxygen‐defective potassium vanadate/amorphous carbon nanoribbons (C‐KVO|O d ) are successfully synthesized through a one‐step solid‐state sintering process as a high‐performance cathode material for ZIBs. This unique 3D interconnected network structure can not only act as a continuous conductive path but also decrease aggregation and provide more adsorption sites for zinc ions. The as‐prepared C‐KVO|O d exhibits a high capacity of 385 mAh g −1 at 0.2 A g −1 , superior rate performance (166 mAh g −1 even at 20 A g −1 ), and an outstanding cycling stability with a 95% capacity retention over 1000 cycles. Density functional theory calculations elucidate that the oxygen defects in the C‐KVO|O d remarkably reduce the Zn 2+ ion's adsorption Gibbs free energy and Zn 2+ ‐diffusion barriers. Meanwhile, the amorphous carbon networks enable the rapid electron transfer and provide additional active sites for Zn 2+ storage. This work can facilitate the development of high‐performance ZIBs for large‐scale energy storage.