The public concerns about agrifood safety call for innovative and reformative analytical techniques to meet the inspection requirements of high sensitivity, specificity, and reproducibility. Enzyme‐mimetic nanomaterials or nanozymes, which combine enzyme‐like properties with nanoscale features, emerge as an excellent tool for quality and safety detection in the agrifood sector, due to not only their robust capacity in detection but also their attraction in future‐oriented exploitations. However, in‐depth understanding about the fundamental principles of nanozymes for food quality and safety detection remains limited, which makes their applications largely empirical. This review provides a comprehensive overview of the principles, designs, and applications of nanozyme‐based detection technique in the agrifood industry. The discussion mainly involves three mimicking types, that is, peroxidase, oxidase, and catalase‐like nanozymes, capable of detecting major agrifood analytes. The current principles and strategies are classified and then discussed in details through discriminating the roles of nanozymes in diverse detection platforms. Thereafter, recent applications of nanozymes in detecting various endogenous ingredients and exogenous contaminants in foods are reviewed, and the outlook of profound developments are explained. Evidenced by the increasing publications, nanozyme‐based detection techniques are narrowing the gap to practical‐oriented food analytical methods, while some challenges in optimization of nanozymes, diversification of recognition‐to‐signal manners, and sustainability of methodology need to conquer in the future.