AM-4 is a layered porous titanosilicate built from TiO6 and SiO4 polyhedra. An improved synthesis of AM-4 crystals enabling control of particle size by secondary growth and reducing synthesis time is presented. A new material, UZAR-S2, has been obtained by exfoliation of the smaller-sized material AM-4. The exfoliation consists of a first stage of proton exchange with acetic acid followed by intercalation with nonylamine and final activation by extraction in HCl/water/ethanol solution. Besides XRD, TEM, N2 adsorption, FTIR and UV-Vis characterization highlighting the delaminated character of UZAR-S2, a potential application regarding CO2 adsorption is also investigated. (© WILEY-VCH Verlag GmbH & Co. KGaA, 69451 Weinheim, Germany, 2009)