Synergy of Multi‐Covalent Bonds Enabling High‐Performance Aqueous Zinc‐Ion Battery Cathodes Toward Industrial‐Grade Mass Loading and Broad‐Temperature Adaptability

ABSTRACT The pursuit of high‐performance cathode materials that are capable of operating reliably under industrially relevant conditions remains a formidable challenge for aqueous zinc‐ion batteries (AZIBs). Here, we tackle this challenge by proposing a novel strategy—synergistic bond engineering—which represents a conceptual advance that departs from conventional approaches. This strategy is materialized in a vanadium oxide cathode, where the deliberate integration of multi‐covalent bonds (O─N─O and N─V) triggers a powerful synergy, enabling efficient operation from baseline to demanding conditions. Through comprehensive simulations and in situ/ex situ characterizations, we elucidate the synergetic mechanism of these bonds: the O─N─O bonds accelerate Zn 2+ diffusion via electrostatic shielding and provide abundant active sites via dynamic reconstruction, while the N─V bonds serve as structural pins that suppress vanadium dissolution and ensure structural integrity. Therefore, the cathode delivers an ultrahigh capacity of 624 mAh g −1 at 0.1 A g −1 and exceptional cycling stability (73% capacity retention after 10 000 cycles at 20 A g −1 ). Crucially, it achieves a record‐high capacity of 504 mAh g −1 under a high mass loading of ≥7 mg cm −2 , along with substantial capacities of 117 and 308 mAh g −1 at 0°C and 60°C, demonstrating the great promise of this “bond‐level” design strategy.