The loss of tissues and organs is a major challenge for biomedicine, and the emerging 3D bioprinting technology has brought the dawn for the development of tissue engineering and regenerative medicine. Chitosan-based supramolecular hydrogels, as novel biomaterials, are considered as ideal materials for 3D bioprinting due to their unique dynamic reversibility and fantastic biological properties. Although chitosan-based supramolecular hydrogels have wonderful biological properties, the mechanical properties are still under early exploration. This paper aims to provide some inspirations for researchers to further explore. In this review, common 3D bioprinting techniques and the properties required for bioink for 3D bioprinting are firstly described. Then, several strategies to enhance the mechanical properties of chitosan hydrogels are introduced from the perspectives of both materials and supramolecular binding motifs. Finally, current challenges and future opportunities in this field are discussed. The combination of chitosan-based supramolecular hydrogels and 3D bioprinting will hold promise for developing novel biomedical implants.