Hydrogels with intrinsic antimicrobial capabilities based on natural strategies have been studied as a hot topic in biomedicine. Nevertheless, it is highly challenging to thoroughly develop a bacteriostatic natural hydrogel. Borneol as a traditional Chinese medicine possesses a unique broad-spectrum antibacterial activity under a membrane-breaking mechanism. In this study, a range of fully natural antibacterial hydrogels are designed and synthesized via the Schiff base cross-linking of carboxymethyl chitosan and dialdehyde dextran grafted natural borneol. The borneol with three configurations is hydrophilically modified onto dextran to boost its antibacterial activity. Also, the synergism of hydrophilic-modified borneol groups and positively charged ammonium ions of carboxymethyl chitosan make the hydrogels totally constrict the E. coli and S. aureus growth during 24 h. Furthermore, the hydrogels exhibit good in vitro cytocompatibility through cytotoxicity, protein adhesion, and hemolytic tests. In view of the injectability, the hydrogels can be delivered to the target site through a minimally invasive route. In short, this work offers a potential tactic to develop antibacterial hydrogels for the treatment of topical wound infections.