Membrane-based separations can lessen the environmental effect of conventional techniques while increasing energy efficiency. Conventional adsorbents, on the other hand, enclose the majority of their functional sites in their dense structures, which causes problems with limited selectivity and adsorption capacity. By top-down method, based on the molecular structure and properties of artemisinin (Ars), a three-dimensional porous basswood membrane and a Metal-organic framework (MOF)-based modified layer were used as a dot-matrix initiator. The combination design of hydrophobic bond and complex bond interaction synergistic imprinting strategy was used to construct high density and high selectivity Ars molecularly imprinted polymers (MIPs) on the membrane, thus achieving the preparation of MOF-initiated imprinted self-supporting basswood membranes (MPIBSMs). When combined with the superhydrophilicity of the TiO2 modified layer and the numerous accessible imprinting sites that MOF previously grown in situ on basswood provided, the resulting MPIBSMs displayed good adsorption capacity (81.2 mg g−1), selectivity coefficient (greater than 4.9), and ultrahigh water flux, eliminating the "trade-off" effect between membrane flux and selectivity. Additionally, the MPIBSMs are synthesized in a straightforward, pollution-free manner. Additionally, MPIBSMs were created in a green way. Finally, the aforementioned experimental findings and the environmentally sound synthetic technique imply that MPIBSMs have a wide range of possible applications in several fields, including environmental protection and selective separation.