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Single‐atom nanozymes (SAzymes) hold great promise in tumor therapy due to their maximized atomic utilization and well‐defined electronic structures. However, they still face challenges of activity, specificity, and targeting that impede therapeutic efficacy. Herein, a practical strategy is reported to construct asymmetric N, S‐coordinated Fe SAzymes (Fe‐S/N‐C). Benefiting from the regulatory influence...