The ordered hexagonal mesoporous materials of Ti-MCM-41 have been synthesized by using the Gemini surfactant bis(hexadecyldimethylammonium bromide)hexane (GEM16-6-16) as template. The X-ray diffraction (XRD) and FTIR results provide the evidence that we can adjust the pore size by varying the Ti/Si ratio. However, there is a limit of Ti/Si ratio favoring the formation of specific structures; the ordered structures will be destructed at higher Ti/Si ratio. The scanning electron micrograph (SEM) and transmission electron micrograph (TEM) images reveal that the Ti-MCM-41 materials exhibit diverse morphologies, including ordered rods, threads and bundles, hexagonal flakes, tubes, discoid rings and helix tubes. We tentatively elucidate that the formation of the complex morphologies can be attributed to the crystal growth mechanism and the defect theory. (C) 2006 Elsevier Ltd. All rights reserved.