Globally, fossil fuel combustion from various industrial processes has caused a significant increase in CO2 emissions, exacerbating the greenhouse effect and climate change. Therefore, effective CO2 capture technologies must be urgently developed. Vacuum temperature swing adsorption (VTSA) is an efficient technique for CO2 capture. The presence of water vapor, H2S, etc., is an important factor that affects the performance of CO2 adsorption, and they are usually removed prior to the adsorption separation process. However, volatile organic compounds (VOCs), a common component of industrial flue gas, can also affect the adsorption and capture of CO2, which is often ignored. Thus, in this study, the effect of isopropanol (IPA), one of the most common VOCs used in industry, on the CO2 removal performance is examined using an in-house VTSA device with activated carbon (AC) as the adsorbent. The effect of IPA on the CO2 adsorption performance of AC under varying IPA concentration, IPA content in AC, feed flow rate, and adsorption/desorption temperature is comprehensively investigated. The results verify that the impact of VOCs in the industrial exhaust gases on CO2 capture by adsorption cannot be disregarded.