Environmentally switched superwetting surfaces that can be used for separating various oil/water mixtures are of particular interest due to the increasing difficulty and complexity in oily wastewater treatment. Here, a novel fluorine-free pH-responsive coating is prepared by surface modification of SiO2 nanoparticles with dimethyloctadecyl [3-(trimethoxysilyl) propyl] ammonium chloride and (N, N-dimethyl-3-aminopropyl) trimethoxysilane. With the assistance of polyethylene imine as a binder, such coating can be used for different porous substrates, e.g. cotton fabric and filter paper, to develop separation materials having tunable superhydrophilicity/superhydrophobicity and high antibacterial property. Due to the well-controlled surface wettability upon the pH variation, the as-prepared materials can effectively separate various types of oil/water mixtures with efficiency higher than 99.9%, including the layered oil/water mixture, water-in-oil emulsions and oil-in-water emulsions stabilized by different types of surfactants. Additionally, the materials can resist strong acid/base solutions and various organic solvents as well as 50-cycle mechanical abrasion and 120-cycle tape-peeling without losing anti-wetting performance. Featuring the tunable surface wettability, chemical/mechanical robustness, and antibacterial activity, such coating holds promising applications for treating various oil/water mixtures in harsh and biological-contamination conditions. (C) 2019 Elsevier Inc. All rights reserved.