Nanostructured films of cadmium hexacyanoferrate (III), Cd-3[Fe(CN)(6)](2) have been deposited on the surface of titanate nanotubes (TiNT) by ion exchange with CdSO4, followed by reaction with K-3[Fe(CN)(6)] in an aqueous suspension. The composite demonstrates a significantly higher hydrogen storage uptake than pure Cd-3[Fe(CN)(6)](2) and TiNT. At a temperature of 77 K and a pressure 100 bar, the hydrogen uptake for the composite is approximately 12.5 wt %, whereas only 4.5 wt % and 4 wt % are achieved for the TiNT and Cd-3[Fe(cN)(6)](2) respectively. Electron microscopy and infrared spectroscopy show that Cd-3[Fe(CN)(6)](2) is uniformly distributed on the surface of the nanotubes forming a discontinuous nanostructured film with a well developed interface, which allows efficient interaction with the support. The possible reasons for the high uptake of hydrogen in the composite are discussed. Copyright (C) 2011, Hydrogen Energy Publications, LLC. Published by Elsevier Ltd. All rights reserved.