Local differences in surface hydrophilicities/hydrophobicities of propyl-and arene-sulfonic- acid modified mesoporous silica and organosilica catalysts have been compared and correlated with their bulk catalytic properties for aqueous-sensitive organic reactions. Syntheses of propyl-and arene-SO3H-modified mesoporous silicas and organosilicas yield materials with different hydrophilicities, especially when ethylsiloxane moieties are ...