Cancer is a worldwide public health issue that has not been conquered. Theranostics, the combination of a therapeutic drug and imaging agent in one formulation using nanomaterials, has been developed to better cure cancer in recent years. Although diverse biomaterials have been applied in cancer theranostics, chitosan (CS), a natural polysaccharide bearing easy modification sites with excellent biocompatibility and biodegradability, shows great potential for developing cancer nanotheranostics. In this review, we seek to describe the chemical functionalities of CS used in cancer theranostics and their synthesis methods. We also present recent discoveries and research progresses on how the CS functionalization could improve the delivery efficiency of CS-based nanotheranostics. Finally, we report several case studies about the application of CS-based nanotheranostics. This paper focuses on the strategies to construct CS-based theranostics systems via chemical routes and highlights their applications in cancer treatment, which can provide useful references for further studies.