Hierarchical structures consisting of microporous titanosilicate TS-1 nanocrystals (MFI-type structure) are obtained by controlled evaporation of colloidal suspensions. The TS-1 nanocrystals with diameter of 60-80 nm are prepared by hydrothermal treatment of clear precursor suspension. The purified TS-1 colloidal suspensions are dried under controlled conditions in order to form hierarchical structures with uniform micropores originated from the TS-1 nanocrystals, mesopores coming from the interparticles spacing and macropores emerging from the controlled evaporation of the solvent. The as-prepared micro/meso/macroporous TS-1 materials are treated by non-thermal plasma to remove the organic template and subsequently characterized by spectroscopy (DLS, IR, UV-vis), microscopy (TEM, SEM), X-ray diffraction, nitrogen sorption and mercury intrusion porosimetry. Besides, the sorption and confinement of 2,4,6-trimethylpyridine (collidine) probe molecule in the micro/meso/macroporous TS-1 structure is followed by FTIR. (C) 2011 Elsevier B.V. All rights reserved.