A　solution　method　for　modifying　thermoplastic　polyurethane　(TPU)　by　the　introduction　of　3D　functionalized　nanohybrids　composed　of　two-dimensional　GONRs　and　one-dimensional　CNTs　was　applied.　FTIR,　XRD,　XPS　and　TEM　were　employed　to　characterize　the　structure　and　properties　of　GONRs-CNTs　hybrids　before　and　after　modification.　The　functionalized　GONRs-CNTs　(pGONRs-CNTs)/TPU　composite　films　were　subsequently　prepared　by　solution　coating　method　on　a　coating　machine.　Furthermore,　by　means　of　oxygen　transmission　rate　test,　tensile　test　and　the　observation　of　surface　morphology,　the　synergetic　effect　between　GONRs　and　CNTs　and　the　effect　of　different　pGONRs-CNTs　content　on　the　barrier　and　tensile　properties　of　TPU　composite　films　were　also　studied.　The　results　show　that　a　unique　three-dimensional　(3D)　crosslinked　nanostructure　is　successfully　obtained,　in　which　GONRs　are　bridged　by　CNTs.　We　also　find　that　the　as-prepared　pGONRs-CNTs　with　neat　shape　and　low　defect　are　evenly　dispersed　in　TPU　matrix　and　form　strong　interfacial　adhesion　with　the　matrix,　while　the　existing　of　CNTs　play　the　role　of　supporting　frame　to　prevent　GONRs　from　sliding　and　aggregation;　modified　by　phenyl　isocyanate,　the　lipophilicity　of　pGONRs-CNTs　composite　is　obviously　improved,　while,　by　the　introduction　of　huge　isocyanate,　the　interlayer　spacing　is　further　improved,　which　is　good　for　uniform　dispersion　in　the　polymer　matrix.　As　a　result,　when　the　mass　fraction　of　pGONRs-CNTs　is　0.5%,　the　barrier　and　tensile　properties　of　pGONRs-CNTs/TPU　composite　films　reach　to　the　optimal　values:　the　oxygen　transmission　rate　decreases　by　63.08%　and　the　tensile　strength　increases　by　46.55%,　compared　with　those　of　the　neat　TPU,　which　will　lead　to　great　benefit　for　the　barrier　and　mechanical　properties　of　TPU　films.　©　2016,　Journal　of　Materials　Engineering.　All　right　reserved.