Due to increasing interest in the development of advanced nanomaterials from nanosheets as building blocks, methods for the preparation of nanosheet materials and their hybrids have been studied carefully and extensively. In this review, studies of mechanochemical methods (solid-solid reactions under ambient conditions or solvent-free synthesis) for the preparation of intercalation compounds are summarized. Mechanochemical reactions without using solvent have operational advantages, such as their environmentally benign nature and the fact that separating and drying the products is not necessary. In addition to their advantages from green chemistry viewpoints, solid-state reactions have potential for the preparation of novel intercalation compounds which are not accessible by conventional solution-based methods.