In this work, we demonstrate the potential of surface-initiated single electron transfer living radical polymerization for surface modification applications that confer low-fouling properties. The versatility of the technique, which can be applied to a wide variety of substrates, has been displayed by the successful grafting of a range of monomers after immobilizing a bromine initiator on the surface via plasma polymerization. The thickness of the grafted surfaces can be controlled through variation of reaction parameters such as monomer concentration, reaction time, and the ratio between catalyst and ligand. Furthermore, the low-fouling properties of the resulting surfaces were demonstrated against fully concentrated serum proteins and adhesive fibroblast cells, via grafting of N-hydroxyethyl acrylamide (N-HEA) or [2-(methacryloyloxy)ethyl]dimethyl-(3-sulfopropyl) ammonium hydroxide (SBMA). This rapid and versatile coating technique, which has the ability to be applied to a wide range of substrates, can be performed in aqueous conditions without the exclusion of atmospheric oxygen, and shows excellent potential for the surface modification of biomaterial surfaces that require low-fouling properties. (c) 2017 Wiley Periodicals, Inc. J. Polym. Sci., Part A: Polym. Chem. 2017, 55, 2527-2536