Aromatic volatile organic compounds (VOCs) are prevalent pollutants in chemically contaminated sites, posing threats to ecological safety and human health. To address the challenge of achieving low-carbon, low-cost, green, and sustainable in-situ remediation at these sites, a highly efficient synthetic bacterial consortium was constructed for biodegradation of selected pollutants (i.e., benzene, toluene, ethyl benzene, m-xylene, chlorobenzene, p-chlorotoluene, and p-chlorotrifluorotoluene). Under optimized conditions, the consortium achieved a total degradation efficiency of 77%. Biodegradation of benzene, toluene, ethyl benzene, and m-xylene followed first-order kinetics, while p-chlorotoluene and p-chlorotrifluorotoluene followed zero-order kinetics. The mechanisms were analyzed using microbiome technology at genetic, protein, and metabolic levels, identifying key enzymes and differences in protein expression and related metabolites. Carbon dioxide measurements and fluorescence spectrum analysis elucidated the transformation pathways. These findings underscore the consortium’s significant potential for achieving effective, eco-friendly, and sustainable bioremediation of aromatic VOCs in chemically contaminated environments.