Mercury is a well-known heavy metal pollutant of global importance, typically found in effluents (lakes, oceans, and sewage) and released into the atmosphere. It is highly toxic to humans, animals and plants. Therefore, the current challenge is to develop efficient materials and techniques that can be used to remediate mercury pollution in water and the atmosphere, even in low concentrations. The paper aims to review the chitosan-based polymer nanocomposite materials that have been used for the environmental remediation of mercury pollution since they possess multifunctional properties, beneficial for the adsorption of various kinds of pollutants from wastewater and the atmosphere. In addition, these chitosan-based polymer nanocomposites are made of non-toxic materials that are environmentally friendly, highly porous, biocompatible, biodegradable, and recyclable; they have a high number of surface active sites, are earth-abundant, have minimal surface defects, and are metal-free. Advances in the modification of the chitosan, mainly with nanomaterials such as multi-walled carbon nanotube and nanoparticles (Ag, TiO2, S, and ZnO), and its use for mercury uptake by batch adsorption and passive sampler methods are discussed.