Boron nitride (BN) has excellent thermal conductivity (TC), however, it exhibits high surface energy, strong chemical inertness, poor interface compatibility with polymer matrices, and difficulty in even dispersion within-polymer matrix, preventive effective construction of TC pathways. Four kinds of modified boron nitride/polyurethane composites (BTPUC) were prepared by different silane-functionalized BN with polyurethane (TPU). Among them, 3-trimethoxysilylpropylmethacrylate (TMSPMA)-functionalized BN demonstrated better interface compatibility with TPU, significantly improving the mechanical properties and TC of the composites compared to the other three functionalized BN addition. The BN@TMSPMA/PU exhibited good TC and mechanical properties, with a TC of 0.865 W/mK, a tensile stress and a tensile strain of 9.65 +/- 1.40 MPa and 759.88 +/- 67.93%, respectively. It also showed good electrical insulation properties and mechanical durability. Therefore, the as-prepared BN@TMSPMA/PU have broad prospects as flexible thermal-management materials.Highlights The composites are constructed by TMSPMA-modified BN and polyurethane by NIPS. The composites show good mechanical properties and cyclic failure resistance. The composites exhibit good thermal conductivity and electrical insulation.