A wide range of trace pollutants persist in aquatic environments, prompting concerns for public health and raising heightened attention. Therefore, the detection of toxic and nonbiodegradable pollutants in aquatic environments at ppm and ppb level is of great significance for measuring waste disposal and monitoring water purity. Among various reported sensors, metal-organic frameworks (MOFs), owning to their customizable structures and adjustable binding sites, have emerged as promising sensing materials in various sensing systems. Herein, this review explores the sensing mechanisms and design strategies for MOF-based fluorescent, electrochemical and photoelectrochemical sensors, followed by noteworthy cases demonstrating their sensitive determination of inorganic anions, metal ions, and organic matter in water. Notably, this review comprehensively summarizes, for the first time, the monitoring performance and sensing system of laboratory-prepared MOFs in real water samples. This comprehensive review may further guide the development of MOF-based sensors and promote their practical applications for sensing aqueous environmental pollutants.