Natural small molecular drugs with excellent biocompatibility, diverse pharmacological activities, and wide sources play an increasingly important role in the development of new drug and disease treatment. In recent years, the utilization of paclitaxel, camptothecin, rhein, curcumin, and other natural small molecular drugs with unique rigid backbone structures and modifiable multiple sites as building blocks to form gels by self-assembly has attracted widespread attention. The obtained low-molecular-weight supramolecular gel not only retains the general characteristics of the gel but also overcomes the shortcomings of natural drugs, such as poor water solubility and low bioavailability. It has the advantages of high drug loading, low toxicity, and outstanding stimulus responsiveness, which is widely used in biomedical fields. Here, we provided a comprehensive review of natural-drugs-based low-molecular-weight supramolecular gels reported in recent years and summarized their assembly mechanism, gel structure, gel properties, and potential applications. It is expected to provide a reference for further research of natural-drugs-based supramolecular gels.