Volatile organic compounds (VOC) are one of the primary pollutants in the atmosphere, mainly from industrial emissions, vehicle exhaust, incomplete fuel combustion, and other processes. The emission of VOCs not only causes harm to air quality and the ecological environment but also seriously threatens human health. Thus, it is highly important to develop environmentally friendly and effective technologies for VOC capture. In recent years, ionic liquids (ILs), a new type of green solvent, have attracted unprecedented attention due to their nonvolatility, high thermal stability, and structural tunability, showing great potential in VOC capture. The designability of ILs enables them to optimize their capture performance for specific VOCs by selecting appropriate cations and anions. This review systematically summarizes the research progress of ILs in capturing different types of VOCs, including the capture mechanisms and application examples of volatile hydrocarbons, oxygencontaining VOCs, chlorine-containing VOCs, sulfur-containing VOCs, and fluorine-containing VOCs. In addition, IL regeneration methods have also been introduced to achieve efficient recycling. Finally, current research challenges and future development directions are summarized and prospected. This review provides a scientific basis for applying ILs in VOC capture and a reference for future research.