Inspired by a surface functional monomer-directing prepolymerization system, a straightforward and effective synthesis method was first developed to prepare highly regenerate and perm-selective molecularly imprinted composite membranes of artemisinin (Ars) molecules. Attributing to the formation of the prepolymerization system, Ars molecules are attracted and bound to the membrane surface, hence promoting the growth of homogeneous and high-density molecular recognition sites on the surface of membrane materials. Afterward, a two-step-temperature imprinting procedure was carried out to prepare the novel surface functional monomer capping molecularly imprinted membranes (FMIMs). The as-prepared FMIMs not only exhibited highly adsorption capacity (11.91 mg g(-1)) but also showed an outstanding specific selectivity (imprinting factor α is 4.50) and excellent perm-selectivity ability (separation factor β is 10.60) toward Ars molecules, which is promising for Ars separation and purification.