The invention relates to a metal-organic framework material for methane adsorption separation and a preparation method thereof. The metal organic framework material is prepared by reaction of at least a metal compound and at least one organic ligand, wherein the metal is one or more selected from Li, Mg, Al, Fe, Co, Ni, Cu, Zn, Mn, Zr, La and Sm, and the organic ligand is one or more selected from single or multidentate organic compounds containing nitrogen, oxygen or sulfur atom. The material has advantages of simple preparation process, high yield, easily available raw materials, mild reaction conditions; besides, the material has stable self properties and porous structure, and is especially suitable for separation of low-quality methane and purification process of high-concentration methane.