Self-supported Ni3S2 ultrathin nanosheets were in situ formed by direct sulfurization of commercially available nickel foam using thioacetamide as sulfur source under hydrothermal process. The morphology and structure of the as-obtained sample were analyzed by using XRD, XPS, SEM, and TEM, revealing that an ultrathin nanosheets Ni3S2 were grown on the surface of Ni form. The as-obtained Ni3S2/Ni composite with uniform architecture was used as cathode material for alkaline Ni/Zn battery, which delivered high capacity of 125 mAh g(-1) after 100 cycles with no obvious capacity fading, extraordinary rate capability (68 mAh g(-1) at the current density of 5.0 A g(-1)), and high operating voltage (1.75 V).