Ti and Ni sulfides were formed on the surface of Ti-Ni alloys by isothermal annealing at various sulfur pressures, and then microstructures of the surface sulfide layers were investigated by means of scanning electron microscopy and X-ray diffractions. Morphology of sulfurized surface changed from granular shape to porous shape at the sulfur pressure of 80 kPa, which is related to the change in sulfide from NiS1.97 to NiS. Two-layered sulfide was observed in which the inner layer was mainly Ti8.2S11, and the outer layer was a mixture of NiS1.97 and NiS. The discharge curve of the Ti and Ni sulfides cathode formed on the Ti-Ni current collector at the first cycle showed a plateau voltage of 1.6 V, and the discharge capacity was found to be about 530 mAb/g-NiS1.97.