Powders press technique is considered as a universal means for preparing cathode of thermal battery. In this work, the flexible NiS2 film cathode with thickness of 120 µm was prepared by tape-casting method. It overcame the issue of organic adhesive failure at high temperature. The NiS2 film retains comparable ductility after heat treatment at 350 °C. And no crack occurs on the surface of the film after 100 times bending. Its density is similar to NiS2 tablets. Assembled in a single thermal battery, an ultrahigh specific capacity of 648 mA h g−1 at 250 mA cm−2 can be achieved with cut-off voltage of 1.5 V. Due to its short lithium ionic transmission distance, the specific capacity increases 13% compared with NiS2 tablets. This work affords a reference significance for the research on full-component flexible thermal battery.