Chronic diabetic wound repair is a global medical challenge. Developing a hydrogel dressing to effectively promote angiogenesis and detect wound state in diabetic wound management is an unmet medical requirement. Herein, a facile and efficient strategy to prepare self-healing hydrogel with enhanced angiogenesis and real-time monitoring for diabetic wounds is presented, by cross-linking carboxymethyl cellulose (CMC) with precoordinated europium-ethylenediaminetetraacetic acid (Eu-EDTA) complexes. Benefiting from the dynamic and reversible coordination interaction formation, the hydrogel exhibits remarkable injectability and self-healing properties, thus forming efficient coverage in irregular and deep wounds with minimally invasive procedures. Furthermore, the fluorescence of the hydrogel changes linearly with pH value in the range of 4.5–7.5 and enables real-time pH measurement to monitor the wound state. More importantly, the hydrogel can effectively promote the proliferation and migration of endothelial cells and enhance tube formation ability, demonstrating great angiogenesis capacity in tissue remodeling. The in vivo experiments manifested that the hydrogel can enhance angiogenesis by upregulating the expression of angiogenesis-related factors and downregulating matrix metalloproteinase-9 (MMP-9), contributing to granulation tissue formation, collagen deposition, and diabetic wound repair. This work can provide a promising strategy for diagnosis and therapy in clinical diabetic wounds.