Environmental pollution is a thoughtful matter around the world because it causes various lethal diseases such as cancer, damage of nervous system, malformation, and angio-cardiopathy. Therefore, rapid, sensitive and cost-effective detection of environmental pollutants is essential for the betterment of life. Recently, metal-organic frameworks (MOFs) have acknowledged miraculous attention to identify the environmental pollutants due to their unique structures and excellent properties. Hence, the author in this chapter systematically presents the key role of MOFs to eliminate the environmental pollutants such as inorganic pollutants (heavy metal and radioactive ions), organic pollutants (organic solvents, antibiotics, pesticides, explosives), and other toxic gases, and volatile organic compounds.