Desertification is one of global environmental problems, which is faced by human beings. Finding a new sand-fixing material is an effective method to combat desertification. In desert areas, water shortage is one of problems that Didymodon vinealis (D. vinealis) grew. In this study, we built up a special-structured nanocomposite. Attapulgite had chain layered crystal structure and many active hydroxyl groups, which made them have high absorption and retention capacity of water. The optimum ratio of dried D. vinealis to attapulgite-based nanocomposite was proved to be 1:4 and the optimum spraying amount 4 mg DW∙cm^-2. The obtained results provided some useful information on the formation of D. vinealis BSCs with the aid of attapulgite-based nanocomposite. In addition, the results would offer a method for the maintenance and management of D. vinealis in desertification control.