Silicone-containing biobased hyperbranched polyurethane thermoplastic elastomers at different compositions were reported for the first time. The structures of the polymers were evaluated from Fourier transform infrared spectroscopy, NMR, X-ray diffraction, and energy-dispersive X-ray spectroscopy analyses. The synthesized elastomers possess high molecular weight (1.11–1.38 × 105 g·mol–1) and low glass transition temperature (from −40.0 to −27.3 °C). These polymers exhibited multistimuli responsive excellent repeatable intrinsic self-healing (100% efficiency), shape recovery (100%), and efficient self-cleaning (contact angle 102°–107°) abilities along with exceptional elongation at break (2834–3145%), high toughness (123.3–167.8 MJ·m–3), good impact resistance (18.3–20.3 kJ·m–1), and adequate tensile strength (5.9–6.9 MPa). Furthermore, high thermal stability (253–263 °C) as well as excellent UV and chemical resistance was also found for the polymers. Most interestingly, controlled bacterial biodegradation under exposure of Pseudomonas aeruginosa bacterial strains demonstrated them as sustainable materials. Therefore, such biobased novel thermoplasticpolyurethane elastomers with self-healing, self-cleaning, and shapememory effects possess great potential for their advanced multifacetedapplications.
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