Zeolites are industrially important materials possessing high Bronsted acidity and shape-selectivity. However, their inherently small pores restrict application for catalytic conversion of bulky molecules. The artificial zeolites have well-tailored Bronsted and Lewis acid sites prepared on mesostructured silica to circumvent this limitation. This novel approach utilizes atomic layer deposition to tailor both porosity and acid speciation, providing exquisite control over catalytic behavior and enabling systematic studies.