A single-step, molecular H 2 -free, integrated catalytic process for producing xylene-rich alkylated aromatics (AAs) using CO 2 as an alkylating reagent has been developed, wherein methylcyclohexane (MCH) is used as a liquid organic hydrogen carrier (LOHC) as well as a reactant, and CO 2 as a carbon source to generate alkylating species. A multifunctional catalyst has been developed through the metal-functionalization of zeolite. Physicochemical properties of the catalyst were studied using characterization techniques, like XRD, FTIR, NH 3 -TPD, pyridine-IR, N 2adsorption−desorption, ICP-OES, UV−vis absorption spectroscopy, HR-TEM, HR-SEM, TGA, etc. The coexistence of Lewis and Bro̷ nsted acid sites in a single catalyst facilitates three types of reaction in a single pass, i.e., the dehydrogenation of MCH to produce toluene and hydrogen, the hydrogenation of CO 2 to form active alkylating species, and the alkylation of toluene to produce AAs. Using LOHC not only sidestepped the storage, transport, and safety issues associated with the molecular H 2 , but also conferred almost four times higher product yield and carbon utilization compared to the molecular H 2 -based process. In a single pass, >70% MCH conversion and ∼58% (wt/wt) selectivity for AAs in the liquid product were achieved, which is equivalent to the space−time yield of ∼390 mg g cat −1 h −1 . The catalyst could effectively suppress the toluene disproportionation and the methanol-to-olefins reaction. The values of reaction free energy calculated using the DFT method indicate that the LOHC-based route is thermodynamically more favorable than the molecular H 2 -based route. Moreover, the in situ utilization of the dehydrogenated species of LOHC as a reactant makes the process atom-economical and evades the process complexity associated with the separation of dehydrogenated LOHC.