Abstract As a powerful tool, nanozyme catalysts broaden the avenues to implement bio‐inspired solutions for addressing many important concerns, covering energy, healthcare, the environment, and more. Recent endeavors, characterized by atomic precision, have enabled extensive exploration of single‐atom nanozymes (SAzymes) with high catalytic activity, superior substrate selectivity, and integrated multifunctionalities, thus becoming an emerging field that bridges nanotechnology and biology. This review provides a brief outline of the progress and summarizes the latest research advances regarding SAzymes in biomedical therapeutics, mainly including tumor therapy, wound antibacterial therapy, and tissue anti‐inflammatory therapy, with a focus on their prototypical synthesis and therapeutic catalytic mechanisms. Finally, current challenges and future perspectives for the engineering of advanced SAzymes are also discussed and outlooked. It is anticipated that this review of the important area shall provide useful guidance for catalytic therapy.