Air is the most crucial and life-supporting input from nature to the living beings of the planet. The composition and quality of air significantly affects human health, either directly or indirectly. The presence of some industrially released gases, small particles of anthropogenic origin, and the deviation from the normal composition of air from the natural condition causes air pollution. Volatile organic compounds (VOCs) are common contaminants found as indoor as well as outdoor pollutants. Such pollutants represent acute or chronic health hazards to the human physiological system. In the environment, such polluted gases may cause chemical or photochemical smog, leading to detrimental effects such as acid rain, global warming, and environmental pollution through different routes. Ultimately, this will propagate into the food web and affect the ecosystem. In this context, the efficient removal of volatile organic compounds (VOCs) from the environment remains a major threat globally, yet satisfactory strategies and auxiliary materials are far from being in place. Metal-organic frameworks (MOFs) are known as an advanced class of porous coordination polymers, a smart material constructed from the covalently bonded and highly ordered arrangements of metal nodes and polyfunctional organic linkers with an organic-inorganic hybrid nature, high porosities and surface areas, abundant metal/organic species, large pore volumes, and elegant tunability of structures and compositions, making them ideal candidates for the removal of unwanted VOCs from air. This review summarizes the fundamentals of MOFs and VOCs with recent research progress on MOF-derived nanostructures/porous materials and their composites for the efficient removal of VOCs in the air, the remaining challenges, and some prospective for future efforts.