Preventing bacterial infections is a crucial aspect of wound healing. There is an urgent need for multifunctional biomaterials without antibiotics to promote wound healing. In this study, we fabricated a guar gum (GG)-based nanocomposite hydrogel, termed GBTF, which exhibited photothermal antibacterial therapy for infected wound healing. The GBTF hydrogel formed a cross-linked network through dynamic borate/diol interactions between GG and borax, thereby exhibiting simultaneously self-healing, adaptable, and injectable properties. Additionally, tannic acid (TA)/Fe3+ nanocomplexes (NCs) were incorporated into the hydrogel to confer photothermal antibacterial properties. Under the irradiation of an 808 nm near-infrared laser, the TA/Fe3+ NCs in the hydrogel could rapidly generate heat, leading to the disruption of bacterial cell membranes and subsequent bacterial eradication. Furthermore, the hydrogels exhibited good cytocompatibility and hemocompatibility, making them a precandidate for preclinical and clinical applications. Finally, they could significantly promote bacteria-infected wound healing by reducing bacterial viability, accelerating collagen deposition, and promoting epithelial remodeling. Therefore, the multifunctional GBTF hydrogel, which was composed entirely of natural substances including guar gum, borax, and polyphenol/ferric ion NCs, showed great potential for regenerating infected skin wounds in clinical applications.