A series of siloxane poly(urethane-urea) (SiPUU) were developed by incorporating a macrodiol linked with a diisocyanate to enhance mixing of hard and soft segments (SS). The effect of this modification on morphology, surface properties, surface elemental composition, and creep resistance was investigated. The linked macrodiol was prepared by reacting α,ω-bis(6-hydroxyethoxypropyl) poly(dimethylsiloxane)(PDMS) or poly(hexamethylene oxide) (PHMO) with either 4,4'-methylenediphenyl diisocyanate (MDI), hexamethylene diisocyanate (HDI), or isophorone diisocyanate (IPDI). SiPUU with PHMO-MDI-PHMO and PHMO-IPDI-PHMO linked macrodiols showed enhanced creep resistance and recovery when compared with a commercial biostable polyurethane, Elast-Eon™ 2A. Small and wide-angle X-ray scattering data were consistent with significant increase of hydrogen bonding between hard and SS with linked-macrodiols, which improved SiPUU's tensile stress and tear strengths. These SiPUU were hydrophobic with contact angle higher than 101° and they had low water uptake (0.7%·w/w of dry mass). They also had much higher siloxane concentration on the surface compared to that in the bulk. © 2018 Wiley Periodicals, Inc. J Biomed Mater Res Part B: Appl Biomater, 107B: 112-121, 2019.
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