Abstract Per‐ and polyfluoroalkyl substances (PFAS) characterized by environmental persistence, bioaccumulation potential, and ecotoxicological risks, have emerged as contaminants of significant global concern in aquatic environments. Accurate and timely detection of PFAS in aqueous systems is essential for effective pollution monitoring, risk assessment, and remediation efforts. Metal–organic frameworks (MOFs), attributing to their ultrahigh surface area, tunable pore architectures, and selective molecular recognition properties, demonstrate exceptional capacity for trace‐level contaminant adsorption and detection, rendering them promising materials for developing high‐performance sensors. This review aims to provide an overview of recent MOFs‐based analytical strategies for PFAS detection, including mass spectrometry, fluorescence detection, surface‐enhanced Raman spectrometry monitoring, and electrochemical sensing. Key aspects addressed include functionalized MOFs for PFAS detection mechanisms, factors affecting PFAS detection, and performance evaluation. Despite substantial progress, challenges remain in translating laboratory‐scale MOFs‐based detection techniques into field‐deployable sensors. These include the need for integrated sampling, preconcentration, and matrix‐tolerant sensing platforms to achieve reliable performance in complex environmental conditions.