Layered double hydroxide (LDH) is a promising drug carrier, ion exchanger, absorbent, and catalyst or even catalyst support due to its inimitable sandwich structure. If the LDH could be synthesized into the nanoscrolls, it will be promising ion channels for the biomolecule transfer, ion exchange, or catalysis. In this report, a simple technique has been developed to prepare layered double hydroxide nanoscrolls on a large scale. The composition of LDH nanoscrolls can be conveniently adjusted through experiment conditions. We proved the "rolling mechanism" to explain the formation of LDH nanoscrolls. Moreover, we unambiguously proposed the driving force for "rolling mechanism", which is the change of the forces between the brucite-like sheets and the interanions and between the cations and cations in the brucite-like sheets. (C) 2006 Elsevier Ltd. All rights reserved.