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Volatile organic compounds (VOCs) have attracted much attention for decades as they are the precursors of photochemical smog and are harmful to the environment and human health. Vacuum ultraviolet (VUV) photodegradation is a simple and effective method to decompose VOCs (ranging from tens to hundreds of ppmV) without additional oxidants or catalysts in the air at atmospheric pressure. In this paper, we review the research progress of VOCs removal via VUV photodegradation. The fundamentals are outlined and the key operation factors for VOCs degradation, such as humidity, oxygen content, VOCs initial concentration, light intensity, and flow rate, are discussed. VUV photodegradation of VOCs mixture is elucidated. The application of VUV photodegradation in combination with ozone-assisted catalytic oxidation (OZCO) and photocatalytic oxidation (PCO) systems, and as the pre-treatment technique for biological purification are illustrated. Based on the summary, we propose the challenges of VUV photodegradation and perspectives for its future development. [Display omitted] [ABSTRACT FROM AUTHOR]