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Nanozymes, nanomaterials exhibiting enzyme‐mimicking activities, have gained considerable interest in biomedicine due to their stability, adjustability, and cost‐efficiency. Among these, metal–organic framework (MOF)‐based nanozymes distinguish themselves by their distinct structure and customizable characteristics. Researchers have explored MOF‐based nanozymes as a platform for developing stimuli‐responsive behaviors. This work first presents the categorization of MOF‐based nanozymes, which are designed to mimic the catalytic functions of oxidases, peroxidases, catalase, superoxide dismutase, hydrolases, and multifunctional enzymes. Crafting MOF‐based nanozymes includes customizing their reactions to particular stimuli, including pH, temperature, light, or biomolecular triggers, ensuring enhanced specificity and potency in catalytic performance amid environmental changes. Moreover, these nanozymes exhibit immense potential in biomedical applications, playing crucial roles in therapeutic interventions like cancer therapy and tissue regeneration. Finally, the article delves into future opportunities and challenges within emerging research frontiers. These stimuli‐responsive MOF‐based nanozymes offer novel avenues for advanced therapeutic strategies, providing prospects for innovative biomedical applications.