A simple method was developed for the preparation of polymeric materials with controlled surface wettability or tunable surface wetting. The method is applicable to a large number of polymers, thermoplastic or thermoset. With this method, it is possible to prepare polymer surfaces with static water contact angles ranging from 0° (superhydrophilic) to greater than 170° (superhydrophobic). The method developed is based on spin-coating of a hydrophilic/hydrophobic silica mixture dispersed in an organic solvent or solvent mixture onto the polymer surface. Depending on the hydrophilic/hydrophobic silica ratio in the coating mixture, it is possible to obtain polymer surfaces displaying gradually changing wettability from superhydrophilic to superhydrophobic. In this article, preparation and surface characteristics of polystyrene (PS) and cross-linked epoxy resin (ER) films are provided as general examples. Polymer surfaces obtained were characterized by scanning electron microscopy, white light interferometry, atomic force microscopy, X-ray photoelectron spectroscopy, and static water contact angle measurements. Effects of the type of polymeric substrate and composition of the silica mixture on the surface behavior of the composite systems were investigated.