Rechargeable aqueous alkaline zinc-based batteries (AZBs) have sparked widespread attention considering their cost-effectiveness, favorable safety profiles, and robust output voltage. Nonetheless, the advancement of AZBs is being constrained by the lack of suitable cathode materials that exhibit high energy storage capacity and great cycle stability. In this work, nickel-cobalt bimetallic selenides (NCS) were synthesized as cathodes for AZBs using a simple one-pot hydrothermal approach, which avoided traditional high-temperature heating procedures, effectively lowering preparation costs, and improving production safety. The optimized sample, NCS-3, presents an impressive capacity of 225.8 mAh g–1 at 1 A g–1 and a satisfactory rate capacity of 194.8 mAh g–1 at an elevated current density of 10 A g–1. In addition, the NCS-3 electrode also achieves long-cycle stability (only 1 % capacity fade after 2000 cycles) and almost 100 % Coulomb efficiency, indicating outstanding structural stability and reversibility. Notably, the NCS-3//Zn battery constructed shows a maximum energy density of 339.3 Wh kg–1, and a power density of 12.5 kW kg–1, highlighting its potential for energy storage applications.