Biomaterials have been widely applied in wound healing since the inception of the biomaterials field. Recent advances in smart biomaterials have led to the development of environment-responsive wound dressings and drug release systems. These materials respond to a variety of stimuli present at the site of a wound, such as reactive oxygen species, cytokines, and enzymes. Selective and precise release of growth factors, anti-inflammatory agents, and/or small molecules in response to the distinct phases of wound healing has been shown to significantly improve the healing process. Furthermore, these advances in controlled delivery have coincided with an increasingly detailed understanding of the wound healing process, creating new and more specific therapeutic targets. This chapter will present an overview of the use of stimuli-responsive smart materials in wound healing by first introducing the sequential phases and biological events in the healing process; second, summarizing key classes of stimuli-responsive materials used in wound healing; and finally, presenting the most recent and promising new directions for the field and offering perspectives for the future.