High biobased carbon content polyurethane dispersions (PUD) are a more sustainable alternative to conventional oil-derived waterborne dispersions in coatings. However, there are still many performance limitations from restricted availability of effective renewable monomers and oligomers. This work demonstrates the improvement of the properties of high biobased content PUD and derived coating by introducing a photo-reversibly crosslinkable coumarin as chain extender within the structure. The effect of partial substitution of 1,3-propanediol biobased by a di-hydroxy photo-reactive cyclic coumarin on the particle size and the stability was analyzed by dynamic light scattering (DLS) and multiple light scattering (MLS). The lateral and more rigid structure of coumarin involved a moderated increment in particle size without significant effect on the dispersion stability for at least 45 days. Associated improvement in hardness and toughness was also demonstrated by tensile test, pendulum hardness, pencil hardness and scratch resistance test. Furthermore, controlled UV irradiation of the polyurethane gave rise to a mechanical performance adjustment from reversible photo-crosslinking and scission of the coumarin molecules within the macromolecular structure. A 70% dimerization degree of the coumarin within the polyurethane film by UV light provided a partially reversible threefold higher tensile strength than that of the original biobased formulation as an effective tool to tune the response of biobased polyurethanes.Graphical