Timely treatment of corneal injuries injury can help to prevent corneal scarring, blindness, and the need for corneal transplantation. This work describes a novel hydrogel that can fill corneal defects and assist in corneal regeneration. This hydrogel is a simultaneous interpenetrating polymer network (IPN) composed of collagen cross-linked via strain-promoted azide-alkyne cycloaddition reaction and hyaluronic acid cross-linked via thiol-ene Michael click reaction. The formation of the IPN gel was confirmed via FTIR spectra, UV-vis spectra, and morphological changes. We compared the gelation time, mechanical properties, transmittance, and refractive index of the IPN gel to the collagen gel, hyaluronic acid gel, and semi-IPN gel. The IPN combined the advantages of collagen and hyaluronic acid gels and supported corneal epithelial cell growth on its surface. When applied to corneal stromal defects in vivo, the IPN avoided epithelial hyperplasia, decreased stromal myofibroblast formation, and increased tight junction formation in the regenerated epithelium.