| Summary: | Anionic waterborne polyurethane (aWPU) is not compatible with graphene oxide (GO) due to the repulsive force acting on identical ionic charges. In this study, we fabricated cationic surfactant treated GO and cationic surfactant treated carbon nanotube (CNT) to increase the compatibility with aWPU. Cationic waterborne polyurethane (WPU) and nanocomposites thereof were also prepared. On the basis of the mechanical properties of the nanocomposites, glass transition temperature (<i>T</i><sub>g</sub>), and a stability test, it was found that the compatibility between WPU and a nanofiller (NF) was enhanced to a great extent when WPU and NF had opposite ionicity. The <i>T</i><sub>g</sub> and mechanical properties of WPU increased with the addition of NF, showed the maximum value and thereafter decreased with further addition. The effect of composition of ionic monomer in WPU was also investigated. As the composition of the ionic monomer increases, the concentration of NF for the maximum <i>T</i><sub>g</sub> and mechanical properties increases. This was attributed to the ionic association between the NF and WPU.
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