Silicones with enhanced protein resistance were prepared by introducing poly(ethylene oxide) (PEO) chains via siloxane tethers (a-c) of varying lengths. Three unique ambifunctional molecules (a-c) having the general formula alpha-(EtO)(3)Si(CH2)(2)-oligodimethylsiloxane(n)-block-poly(ethylene oxide)(8)-OCH3 (n = 0 (a), 4, (b), and 13 (c)) were prepared via regioselective Rh-catalyzed hydrosilylation. Nine films were subsequently produced by the H3PO4-catalyzed sol-gel cross-linking of a-c each with alpha,omega-bis(Si-OH)polydimethylsiloxane (P, M-n = 3000 g/mol) in varying ratios (1: 1, 1:2, and 2:3 molar ratio a, b, or c to P). Films prepared with a 2:3 molar ratio (a-c to P) contained the least amount of un-cross-linked materials, which may migrate to the film surface. For this set of films, surface hydrophilicity and protein resistance increased with siloxane tether length (a-c). These results indicate that PEO was more effectively mobilized to the surface if incorporated into silicones via longer siloxane tethers.