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Abstract: The current paper reports the synthesis of a highly hydrophilic, antifouling dendronized poly(3,4,5-tris(2-(2-(2-hydroxylethoxy)ethoxy)ethoxy)benzyl methacrylate) (PolyPEG) brush using surface initiated atom transfer radical polymerization (SI-ATRP) on PDMS substrates. The PDMS substrates were first oxidized in H2SO4/H2O2 solution to transform the Si–CH3 groups on their surfaces into Si–OH groups. Subsequently, a surface initiator for ATRP was immobilized onto the PDMS surface, and PolyPEG was finally grafted onto the PDMS surface via copper-mediated ATRP. Various characterization techniques, including contact angle measurements, attenuated total reflection infrared spectroscopy, and X-ray photoelectron spectroscopy, were used to ascertain the successful grafting of the PolyPEG brush onto the PDMS surface. Furthermore, the wettability and stability of the PDMS–PolyPEG surface were examined by contact angle measurements. Anti-adhesion properties were investigated via protein adsorption, as well as bacterial and cell adhesion studies. The results suggest that the PDMS–PolyPEG surface exhibited durable wettability and stability, as well as significantly anti-adhesion properties, compared with native PDMS surfaces. Additionally, our results present possible uses for the PDMS–PolyPEG surface as adhesion barriers and anti-fouling or functional surfaces in biomedical applications. [Copyright &y& Elsevier]