This chapter focuses on the application of membrane technology in the field of Volatile Organic Compounds (VOCs) separation and desulfurization. The diverse types of VOCs separation membranes, including VOC sieving membranes and preferential permeable membranes, are discussed. Sieving membranes are primarily utilized for VOC retention, while preferential permeable membranes emphasize the permeation of specific VOCs. The preparation methods of membranes involve material selection and processing, and their performance parameters such as permeability flux and selectivity are crucial indicators for evaluating membrane performance. Additionally, the membrane mass transfer models, encompassing the transport mechanisms of porous and dense membranes, are highlighted. The selection and characteristics of membrane materials play a pivotal role in membrane-based desulfurization. Different types of desulfurization membranes, such as hydrophobic and hydrophilic membranes, possess unique desulfurization mechanisms. The preparation methods of membranes also influence their performance, and the performance parameters serve as the key for assessing desulfurization efficacy. The mass transfer models of hydrophobic and hydrophilic desulfurization membranes exhibit distinct characteristics. Overall, membrane technology provides a novel approach for VOCs separation and desulfurization. Compared to traditional techniques, membrane-based methods offer advantages in efficiency and environmental friendliness, though their practical performance requires further validation and optimization.