Microspheres are a new type of drug carrier with great potential for development and application. Natural polymers have good biocompatibility, biodegradability, and are easily dispersed in living organisms, making them suitable for preparing microspheres. Inorganic materials (mainly inorganic minerals) have excellent mechanical properties and are inexpensive and easy to obtain. Through the coupling and hybridization of natural polymers and inorganic materials, they can complement each other's advantages and synergistically enhance efficiency, resulting in many excellent physical and chemical properties. Inorganic materials/natural polymer composite microspheres can be prepared by modifying natural polymers with inorganic materials through various methods such as emulsification crosslinking, solution mixing, in-situ synthesis, extrusion, etc. The application of inorganic materials/natural polymer composite microspheres in drug delivery systems has significant sustained-release effects, is safe and non-toxic, and the cost of carrier materials is relatively low, which has certain significance for the development of new drug carriers. This article reviews the recent research on the preparation, drug loading and release properties of inorganic material/natural polymer composite microspheres, analyzes the advantages and disadvantages of commonly used preparation methods, and looks forward to the development direction of composite microspheres.