A metal sulfide single crystal material comprises metal element M and sulfur element S; the chemical formula thereof is MSx, wherein x is not more than 3 and not less than 1, the metal elements are In, Sn, Sb, Ti, V, Mo, Mn, Co, Cu or Zn; the material is prepared with a method in combination with high energy ball milling method and high temperature solid phase method, comprising the following steps: mixing the sulfur powder with metal powder, and placing in a ball mill tank to carry out ball milling in argon atmosphere; thermostatically baking at low temperature and high temperature for a long time in the argon atmosphere and mixed atmosphere of argon atmosphere and air; cooling, and repeating the steps of 2-6. The preparation method uses simple device, the process conditions are simple and easy, the production cost is low, and the process is environment-friendly and is suitable for production in a large scale. The material can be widely applied to the fields such as high temperature lubricant, hydrogenation catalyst, high energy power supply, hydrogen storage material, semiconductor material, or even super conductive material.