† Electronic Supplementary Information (ESI) available: FTIR spectra, Raman spectrum, 1 H NMR spectra, UV-visible spectra, mass spectrum, HPLC spectra, DSC heating curves, tensile stress-strain curves, effect of exposure time of xenon lamp light on Young's modulus, and tabulated mechanical properties and healing efficiencies. See For realizing sunlight stimulated self-healing, a crosslinked polyurethane carrying disulfide in the main chain is synthesized. Its macromolecular composition and architecture are optimized so that the included disulfide bonds can take part in exchange reaction simply under illumination of the low concentration UV component of sunlight. Accordingly, the damaged polymer is allowed to be repeatedly healed in the sun in terms of strength restoration as a result of phototriggered reversible exchange of disulfide bonds. Meanwhile, the elaborately introduced hydrogen bonding helps to quickly close crack, favoring intimate contacts of cracked surface and subsequent interaction of dangling chains across the interface, and eventually raising effectiveness of photo-reaction of the disulfide bonds in solid phase. In addition, networks rearrangement due to disulfide exchange enables multiple recycling and reshaping of the polymer under sunshine. The present proof-of-concept work would be hopefully developed into a cost-effective and environmentally friendly technology of design, fabrication and application of smart photo-sensitive polymer with higher mechanical strength.