In this paper, a mechanochemical approach is used to prepare layered double hydroxides (LDHs). This approach involves manually grinding the precursor, nitrates and then the hydrothermal treatment. The study indicates that grinding leads to the incomplete formation of LDHs phase, LDHs-M. The reaction degree of precursor salts to LDHs after grinding depends on the melting points of the precursors. As expected, hydrothermal treatment is beneficial for the good crystallization and regularity of LDHs. Especially, the effect of hydrothermal treatment has been emphatically explored. The hydration of LDHs-M, increment of zeta potentials and the complete exchange of NO3- by CO32- anions occur successively or in parallel during the hydrothermal treatment. It can be found that combination of grinding and hydrothermal treatment gives rise to the formation of uniform and monodispersed particles of LDHs. (C) 2013 Elsevier B.V. All rights reserved.