In this work, a series of polyurethane/montmorillonite (PU/MMT) nanocomposite films were prepared by in-situ polymerization method. The effect of MMT contents on the properties of the films was investigated using various test methods. MMT enhanced the thermal stability of the films, and the glass transition temperature of PU/MMT films was increased because MMT limited the movement of molecular chains of PU. MMT was well-dispersed in the nanocomposites because the agglomeration of MMT was inhibited by mechanical force. Especially in the PU/4% MMT nanocomposite, MMT showed the best dispersibility. This study showed that the addition of MMT effectively improved the properties of the PU/MMT nanocomposite films.