Graphical Abstract: Mesoporous silicas with the thiourea functional group ≡Si(CH2)3NHC(S)NHC2H5 have been synthesized by monotemplate and bitemplate route (bitemplate is cetylpyridinium chloride as micelle-forming surfactant and monoethanolamide of saturated n-aliphatic acid as non-micelle-forming surfactant). The infl uence of a number of factors on mesoporous silicas structure has been studied: alkoxysilanes and surfactants concentration, and as well as the nature of medium in hydrothermal treatment of mesophases. The optimum conditions under which functionalized mesoporous silicas have possessing highly ordered hexagonal structure have been found. The surface area of mesoporous silicas synthesized using optimum bitemplate solubilization composition reaches 1055-1350 m2/g and sorption volume and pore diameter are 0.75-0.95 cm3/g and 2.5-2.9 nm respectively.