Abstract: A novel method was adopted to modify TPU with the nanohybrids consisting of two-dimensional graphene oxide nanoribbons (GONRs) and one-dimensional carbon nanotubes (CNTs). The GONRs-CNTs nanohybrids were obtained with a weight fraction of GONRs of 67 wt % through oxidative longitudinal unzipping for MWCNTs, followed by a modification with phenyl isocyanate. The functionalized GONRs-CNTs (pGONRs-CNTs)/TPU composite films were then prepared by a solution coating method using a coating machine. The effect of pGONRs-CNTs content on the barrier, tensile and degradation properties of the composite films was investigated. The results indicated that pGONRs-CNTs were well dispersed in the TPU matrix with a neat shape and low defect due to its strong interfacial adhesion with TPU. When 0.5 wt % of pGONRs-CNTs was incorporated into TPU, the composite films achieved the optimium barrier and tensile properties, in which the oxygen transmission rate decreased by 63.08 % and the tensile strength increased by 46.55 % compared to those of pure TPU film. In addition, the addition of pGONRs-CNTs also improved the serving time of the composite films.