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Structural adhesives are bonding materials that can quickly join structures with components and repair cracks. However, thermosetting polyurethane structural adhesives suffer from disadvantages such as insufficient toughness, poor aging resistance, and long curing time, which greatly limit their practical application. Herein, a polyurethane (PU) composite with excellent mechanical properties was prepared successfully via regulating the cross-linking structure and the dispersion of core-shell-rubber (CSR) particles. Various polyols were selected to improve the cross-linking density of the PU and to enhance the intermolecular forces, which can achieve the high strength and stability of the polyurethane composites. Solvent displacement was used to improve the dispersion of CSR in PU. The cured composite has ultra-high toughness and impact resistance due to the well-dispersed CSR particles. The impact strength was increased from 52.0 to 90.4 kJ/m2, and the elongation at break was increased from 6.1% to 14.9%. Due to the addition of catalyst T120, this composite can be cured quickly at room temperature, reaching high strength after 30 min. In addition, these composites can resist extreme environments, such as high and low temperature changes, UV aging, high humidity and heat environment, and salt spray aging, which has potential and value for practical application. The prepared PU structural adhesive can meet the requirements of structural bonding transit and improve the production efficiency. This work proposed a novel strategy to prepare polyurethane composites with excellent mechanical properties for structural adhesive application. [ABSTRACT FROM AUTHOR]