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Nanocomposites based on waterborne polyurethane (WPU) and graphene oxide (GO) have been synthesized and characterized. It was found that after the incorporation of GO, WPU films became mechanically more rigid, and the Young’s modulus increased by almost six times. It is shown that the lateral size of GO sheets influences the mechanical properties of WPU/GO composites. In particular, composites with larger lateral size of GO sheets have higher values of Young’s modulus. Additionally, if the mechanical properties are improved with the addition of GO additive, then water absorption decreases for WPU modified with small GO sheets whereas it increases for WPU modified with large GO sheets. Possible reasons for this behavior are discussed.