In recent years, polyurethane nanocomposites have attracted more attention due to the massive demand for materials with increasingly exceptional mechanical, optical, electrical, and thermal properties. As nanofillers have a high surface area, the interaction between the nanofiller and the polymer matrix is an essential issue for these materials. The main aim of this study is to validate the impact of the montmorillonite nanofiller (MMT) surface structure on the properties of polyurethane thin-film nanocomposites. Despite the interest in polyurethane–montmorillonite clay nanocomposites, only a few studies have explored the impact of montmorillonite surface modification on polyurethane’s material properties. For this reason, four types of pol...