In order to enhance the controlled-release property of starch-based polyurethane (SPU) coating, polyurethane/montmorillonite (SPU/MMT) composite coatings for controlled-release urea were prepared by in-situ polymerization with a rotating drum. The effect of MMT on morphology, structure, physicochemical properties, especially controlled-release property of the as-prepared composite coatings were studied in detail. The results showed that MMT particles dispersed well in SPU matrix, and the obtained SPU/MMT composite coatings possessed more tough and compact morphology with less-visible holes compared with SPU coating. With the content of MMT rising to 3%, the time needed for 75% nitrogen release increased to 49 days, much longer than 14 days of SPU coating. Further, the nitrogen release mechanism underlying the structure and properties of SPU/MMT composite coatings were discussed and elucidated. According to the analysis, the superior controlled-release prop-