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Veratraldehyde is an important chemical used in perfumery, agrochemical, and pharmaceutical industries. Current processes of manufacture of veratraldehyde use homogeneous catalysts, which make them highly polluting, creating problems of disposal of effluents and product purity. In the current work, veratraldehyde was synthesized from O-alkylation of vanillin with an environmentally benign reagent, dimethyl carbonate. A series of potassium loaded La2O3–MgO were prepared by the incipient wetness impregnation method, and their performance was evaluated vis-à-vis MgO, La2O3, La2O3–MgO, and a series of 1–4 wt % K/La2O3–MgO. All catalysts were characterized by different techniques, such as N2 adsorption/desorption, XRD, TGA-DSC, FT-IR, CO2-TPD, and SEM techniques. The effect of different loadings (1–4 wt %) of potassium on La2O3–MgO was studied, among which 2 wt % K/La2O3–MgO showed the best activity and selectivity due to high dispersion of potassium and high basicity in comparison with the rest. The activity of 2 wt % K/La2O3–MgO in O-methylation of vanillin with dimethyl carbonate (DMC) was closely associated with basicity. Various parameters were studied to achieve the maximum yield of the desired product. The maximum conversion was found with catalyst loading of 0.03 g/cm3 and mole ratio of vanillin and DMC of 1:15 at 160 °C in 2 h. The reaction follows pseudo-first-order kinetics for the O-methylation of vanillin. The energy of activation was found to be 13.5 kcal/mol. Scale-up was done using the kinetic model to observe that the process could be scaled up using the process parameters. The overall process is clean and green.

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