AbstractAqueous rechargeable Zn‐metal batteries (AZMBs) are promising energy storage aids due to their inherent safety, low cost, and competent performance, with prospects in stationary and portable applications. In this regard, one of the critical requirements is developing electrodes that can adapt to mechanical deformation without compromising the charge storage performance. The current work demonstrates the development of a binder‐free and mechanically flexible composite cathode film (VP/fCNT‐F, where ‘F’ stands for the film) based on VOPO4 (VP) and functionalized carbon nanotubes (fCNTs). The VP/fCNT‐F film processing involves simple vacuum filtration of the composite obtained from the in‐situ reaction of the fCNTs and the VP precursor in an aqueous medium. The functionalization of carbon nanotube (CNT) is important for the homogenous dispersion of VP and fCNT. The VP/fCNT‐F electrode is used as a monolithic electrode in AZMB cells in combination with both liquid and quasi‐solid‐state gel polymer electrolytes. Besides, the utility of the VP/fCNT‐F electrode in a flexible battery configuration is also demonstrated. Interestingly, in both the coin‐cell and flexible configurations, the VP/fCNT‐F electrode delivers a comparable discharge capacity of 90 and 78 mAh g−1, respectively (at 0.1 A g−1), validating the advantage of the binder‐free VP/fCNT‐F electrode for AZMBs.

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