A microporous pH- and light-responsive membrane that enables remote control over its interfacial properties has been fabricated. pH-Responsiveness was imparted to a porous polypropylene film via grafting of poly(methacrylic acid) brushes from the substrate using argon-plasma-induced free-radical graft polymerization. Morphological changes as a function of grafting level were analyzed using atomic force microscopy. Conversion into a light-responsive membrane was performed via postpolymerization modification to covalently attach photochromic spiropyran moieties to the grafted polymer brushes. Reversible switches in wettability and permeability were determined upon changing from acidic to basic pH or upon alternating UV- and visible-light irradiation. Additionally, light-responsive membranes show a switch in color upon UV exposure.