With rapidly increasing environmental pollution, there is an urgent need for the development of fast, low-cost, and effective sensing devices for the detection of various organic and inorganic substances. Silver nanoparticles (AgNPs) are well known for their superior optoelectronic and physicochemical properties, and have, therefore, attracted a great deal of interest in the sensor arena. The introduction of AgNPs onto the surface of two-dimensional (2D) structures, incorporation into conductive polymers, or within three-dimensional (3D) nanohybrid architectures is a common strategy to fabricate novel platforms with improved chemical and physical properties for analyte sensing. In the first section of this review, the main wet chemical reduction approaches for the successful synthesis of functional AgNPs for electrochemical sensing applications are discussed. Then, a brief section on the sensing principles of voltammetric and amperometric sensors is given. The current utilization of silver nanoparticles and silver-based composite nanomaterials for the fabrication of voltammetric and amperometric sensors as novel platforms for the detection of environmental pollutants in water matrices is summarized. Finally, the current challenges and future directions for the nanosilver-based electrochemical sensing of environmental pollutants are outlined.