Molecular layer deposition (MLD) for the deposition of polyimide (PI) at low temperature of 110 degrees C has been firstly introduced into the field of membrane separation. With the optimized MLD deposition parameters, such low deposition temperature has successfully expanded the application of MLD for the surface modification of polymeric materials. Globular PI particulates grow on both the free surfaces as well as the pore walls of the polypropylene (PP) membranes as isolated islands during progressive precursor exposures. The PI-deposited PP membranes exhibit synergistically improved performances in various aspects. Evidently improved surface hydrophilicity and permeation performance (30%) have been achieved via the MLD deposition of polyimide films. The overall separation efficiency maintained higher than 85% even after 250 cycles of MLD deposition. More importantly, the thermal stability has been improved and the integrity of the porous structure for PI-deposited PP membranes has been well preserved even after harsh treatment, which ensures its potential application in industries. (C) 2016 The Chemical Industry and Engineering Society of China, and Chemical Industry Press. All rights reserved.