Compared with Zn, the current mainly reported charge carrier for zinc hybrid capacitors, small-hydrated-sized and light-weight NH is expected as a better one to mediate cathodic interfacial electrochemical behaviors, yet has not been unraveled. Here we propose an NH-modulated cationic solvation strategy to optimize cathodic spatial charge distribution and achieve dynamic Zn/NH co-storage for boosting Zinc hybrid capacitors. Owing to the hierarchical cationic solvated structure in hybrid Zn(CFSO)-NHCFSO electrolyte, high-reactive Zn and small-hydrate-sized NH(HO) induce cathodic interfacial Helmholtz plane reconfiguration, thus effectively enhancing the spatial charge density to activate 20% capacity enhancement. Furthermore, cathodic interfacial adsorbed hydrated NH ions afford high-kinetics and ultrastable C‧‧‧H (NH) charge storage process due to a much lower desolvation energy barrier compared with heavy and rigid Zn(HO) (5.81 vs. 14.90 eV). Consequently, physical uptake and multielectron redox of Zn/NH in carbon cathode enable the zinc capacitor to deliver high capacity (240 mAh g at 0.5 A g), large-current tolerance (130 mAh g at 50 A g) and ultralong lifespan (400,000 cycles). This study gives new insights into the design of cathode-electrolyte interfaces toward advanced zinc-based energy storage.