However, due to the use of water as the dispersion medium and abundant hydrophilic moieties of the molecular skeleton, waterborne polyurethanes always suffer from poor mechanical properties and inferior water resistance. In this work, dehydrated sorbitan monooleate (SP), a bio-derived renewable polyol, is introduced into the waterborne polyurethane skeleton to modulate the contents of the traditional trifunctional polyol of trimethylolpropane (TMP). Due to the rigid furan ring and the fatty side chain in the SP, the SP-modulated waterborne polyurethanes (WPU-SP) exhibit simultaneous excellent mechanical properties, high toughness, flexibility, and versatility, with the maximum tensile strength of WPU-SP reaching 39.19 MPa, and the film is capable of lifting weights over 25,000 times its own weight without fracture.