A novel hierarchically heterostructured TiO2 nanocomposite, which consists of rutile nanosheets perpendicular standing on anatase nanofibers, is successfully created through a two-step approach. Firstly, the fibrous anatase TiO2 framework is fabricated by a facile electrospinning method, then a layer of relative uniform rutile nanosheets grow on the fibers after a mild solvothermal reaction process. This work provides a convenient and effective route for fabricating desired three-dimensional nanocomposite and should be easily extended through to many other materials system. (C) 2010 Elsevier Masson SAS. All rights reserved.