Once cracks have formed within hydrogel materials, the integrity of the structure is signifcantly compromised, regardless of the application. Here, we demonstrate cross-linked CMCS hydrogels can be engineered to exhibit self-healing under mild conditions. CMCS hydrogels based on CMCS and acryloyl-6-aminocaproic acid (A6ACA) were synthesized by free radical aqueous copolymerization using ammonium persulfate as initiator. A series of hydrogels was synthesized varying the percentage of A6ACA. The hydrogels were characterized by Fourier transform infrared spectroscopy (FTIR) techniques and their morphologies were investigated by scanning electron microscope (SEM) images. When the proportion of A6ACA was increased, the compressive strength, stress, and strain of hydrogels were increased. The cross-linked hydrogel based on CMCS that can autonomously heal between cut surfaces after 1 h was formed under mild conditions. The increase of A6ACA content in the hydrogels will lead to increased mechanical properties and mechanical healing efficiencies for highly cross-linked polymeric networks. Hydrogen bond is the main reason for self-healing ability, and the covalent cross-linkss and noncovalent cross-links both bear loads in the hyrogel. Polymers with the ability to self-repair after sustaining damage could extend the lifetime of materials used in many applications.