A modified oil-drop sol-gel process is reported for synthesis of mesoporous spherical gamma-Al2O3 granular particles and CuO-coated gamma-Al2O3 granular particles of 1-3 mm in diameter. Various parameters affecting the granulation process were studied, and the optimum values of these parameters were identified for reproducible synthesis of the alumina granular particles. Under the optimum synthesis conditions, CuO-coated gamma-Al2O3 granular particles could be synthesized directly from the pseudo-boehmite sol doped with Cu(NO3)(2) by a solution-sol mixing method. The CuO-coated gamma-Al2O3 granular particles prepared by the solution-sol mixing coating method exhibit better mechanical and sulfation properties than the similar sorbents prepared by the wet-impregnation method. The sol-gel derived granular CuO-coated gamma-Al2O3 sorbents prepared by both coating methods have the same microstructure at lower CuO loading.