Abstract: A three-dimensionally ordered macroporous (3DOM) metal-organic framework material (MOF)-based quasi-solid-state electrolyte thin film for a safe quasi-solid-state lithium secondary battery are provided by the present invention. In detail, the above quasi-solid-state electrolyte combines 3DOM-MOFs and the electrolytes like polymer and traditional liquid electrolyte. The special pore structures in 3DOM-MOFs could both fill the polymer electrolyte and liquid electrolyte with macropores and micropores, respectively. This unique structure could significantly enhance the Li+ conductivity rate through the different kinds of electrolytes in the corresponding pore structures as well as improve the battery performance. More importantly, this quasi-solid-state electrolyte is much safer than the traditional organic electrolyte. It should be easy to scale-up since the procedures are simple.