Metal organic framework (MOF) crystal films have attracted much attention in the field of gas separation due to their pore structure regulation at molecular level. However, the preparation of high quality MOF gas separation film has always been a challenge due to many grain boundary defects and the difficulty of film formation. Therefore, a solution to prepare MOF crystal-glass composite film was proposed in this paper, taking advantages of MOF glass without grain boundary and easy forming. Firstly, ZIF-8/ZIF-62 crystal film with mixed crystal composite and double layer composite was prepared by in-situ solvothermal method, and then the crystal-glass composite film was prepared by melting and cooling. The results show that the fused ZIF-62 liquid phase can effectively bridge the grain boundary defects and make film dense. Compared with mixed crystal films, the crystal-glass composite films prepared by ZIF-8/ZIF-62 multilayer composite films have higher gas selectivity and separation efficiency for H₂/N₂, H₂/CH₄, CO₂/N₂, and CO₂/CH₄ mixed gases. Especially for H₂/CH₄ and CO₂/CH₄, the selectivity can reach 27.7 and 26.5, respectively.