This study explores the sensing capabilities of chemical vapor deposition (CVD)-grown graphene in detecting volatile organic compounds (VOCs) through quartz crystal microbalance (QCM) and surface plasmon resonance (SPR) techniques. Two distinct sensing devices were developed, each tailored for QCM and SPR transducing mechanisms, utilizing CVD graphene as the sensing element. The sensors demonstrated consistent and reproducible responses when exposed to various concentrations of dichloromethane, chloroform, carbon tetrachloride, benzene, toluene, and m-xylene. Notably, both sensors exhibited unparalleled sensitivity to dichloromethane, with the graphene-coated SPR sensor displaying a sensitivity value of 294 × 10−3 ppm−1 and a limit of detection (LOD) value of 10.62 ppm. Additionally, the SPR sensor showcased remarkably swift response and recovery times, both under 3 sec. Results indicate that the adsorption of VOC molecules on the CVD graphene surface increases with the rising dipole moments and vapor pressure values of the molecules. The utilization of CVD graphene in both sensing approaches demonstrates good reproducibility in detecting ultralow concentrations of VOCs at room temperature.