An attractive strategy involving photodimerization of a novel amidocoumarin moiety is presented to prepare polyurethane coatings with excellent mechanical properties. Two families of polyurethanes containing these chromophore units into soft or hard segments were easily synthesized by inserting a small fraction of amidocoumarin-diol (5 wt% or 10 wt%). A systematic study has been carried out comparing hard segment, chromophore content and the influence of this amidocoumarin unit within the hard or soft segment. For all synthetized polymers, mechanical properties of the coatings have been evaluated before and after an excitation of the coumarin units with UV light. The results show that the insertion of coumarin into the hard segment leads to a considerable improvement of the mechanical properties after irradiation. Additionally, the photochemical activity of amidocoumarin was studied by UV-Vis and Raman spectroscopies.