Synthetic polymer membranes are widely used in many applications, including, among others, water purification, protein separation, and medicine. However, the use of existing polymer membranes faces major challenges, such as the trade-off between permeability and selectivity, membrane fouling, and poor mechanical strength. To address these problems the authors have focused their research on surface/interfacial tailoring and the structure-property relationship of polymer membranes used in liquid separation systems. Progress has been made as follows: (1) a methodology for membrane surface functionalization and nanofiltration (NF) membrane preparation based on mussel-inspired catecholic chemistry was proposed and established; (2) a class of mechanically robust and environmentally-responsive composite membranes with hydrogel pore-filled in rigid macroporous supports was designed and developed; (3) a methodology for surface tailoring and antifouling modification of polymer membranes based on amphiphilic copolymers was created and the scientific implications for amphiphilic polymer membranes elaborated; (4) an adsorption membrane with both filtration and adsorption functions was designed and developed to achieve rapid removal of trace micropollutants, including heavy metal ions, organic dyes, plasticizer, antibiotics, and others. This mini-review briefly summarizes this work.