In spite of the intense efforts in selective separation field, the utilization and preparation of membrane-associated molecularly imprinted membranes with both enhanced rebinding capacities and high permselectivity performance still remain strong challenges. Herein, the bioinspired PDA-modified porous regenerated cellulose membrane (pRCMs) with mineral-coated multilevel structure was first proposed for the preparation of PDA/CaCO3-based imprinted nanocomposite membranes (PCIMs), m-cresol was chosen as the template molecule. Importantly, this bioinspired methodology was redeveloped and optimized to obtain abundant and uniformly distributed CaCO3 nanocomposite on the surfaces of PDA@pRCMs. The as-designed sandwich-like imprinting structure were then constructed on PDA/CaCO3-based surfaces by developing a simple sol-gel imprinting process. Attributing to the design of the uniform CaCO3/PDA@pRCMs surfaces, amount of m-cresol-imprinted sites and permeation selectivity could be both optimized, it was no surprise that more excellent rebinding capacity (97.4 mg g(-1)), fast adsorption kinetics and high permselectivity coefficients (more than 13) were successfully achieved. Importantly, the whole synthesis process was conducted without complicated procedures and polluting the environment. Finally, the experimental results mentioned above, together with the green synthesis processes strongly demonstrated that our synthesis methodology of PCIMs had great potential for applications in various fields of selective separation, chemical industry, environment, biological medicine and so on. (C) 2020 Elsevier Inc. All rights reserved.