Natural polymers have been particularly appealing for constructing hemostatic materials/devices, but it is still desirable to develop new natural polymer-based biomaterials with balanced hemostatic and wound-healing performance. In this work, a natural polyphenol-functionalized chitosan/gelatin sponge (PCGS) was prepared by the lyophilization of a chitosan/gelatin mixture solution (under a self-foaming condition to prepare the CGS) and subsequent chemical cross-linking with procyanidin (PC). Compared with the original CGS, PCGS exhibited an enhanced liquid-absorption ability, reduced surface charges, and similar/low hemolysis rate. Benefiting from such a liquid-absorption ability (∼4000% for whole blood and normal saline) and moderate surface charges, PCGS exhibited high in vitro hemostatic property and promising hemostatic performance in an in vivo femoral-artery-injury model. In addition, PCGS possessed higher antioxidant property and slightly decreased antibacterial ability than CGS, owing to the incorporation of PC. The feasibility of PCGS for treating infected wounds was further confirmed in an in vivo infected-tooth-extraction model, as the typical complication of intractable tooth-extraction bleeding. The present work demonstrated a facile approach for developing multifunctional hemostatic materials through the flexible management of natural polymers and polyphenols.