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Firstly, GO was modified by isophorone diisocyanate (IPDI). GO was successfully grafted with isocyanate (-NCO) by FTIR. Then, in-situ polymerization was used to react polytetramethylene ether glycol 1000 (PTMG 1000) with —NCO on modified GO (IGO), and then prepolymerized with diphenylmethylene diisocyanate (MDI) to prepare IGO @ thermoplastic polyurethane elastomer (TPU) nanocomposites. As a comparison, GO was added during the pre polymerization of MDI and PTMG 1000, and GO/TPU composite materials were prepared by solution blending method. The results indicated that, compared to GO/TPU and pure TPU, IGO@TPU had better mechanical properties. The tensile strength and elongation at break of IGO@TPU were 36 MPa and 570.5% respectively, which increased by 338% and 70.6% compared with TPU and 188% and 61.5% compared with GO/TPU.