Hydrotalcite-like compounds of the formula NixZn6-xAl2(OH)(16)(SO4)(.)4H(2)O where x varies from 0 to 6, equivalent to a zinc-substituted carrboydite have been synthesised and characterised by X-ray diffraction, electron microscopy and vibrational spectroscopy. Both the d (003) spacing and the crystallite size are a function of the amount of zinc replacement for nickel in the carrboydite-like compounds. Transmission electron microscopy (TEM) shows the clay-like crystal structure for these hydrotalcite compounds. These compounds were characterised by vibrational spectroscopic techniques and a comparison made with the naturally occurring minerals. Additional bands in the sulphate antisymmetric stretching and bending region leads to the conclusion that the symmetry of the sulphate anion is reduced inferring the bonding of the sulphate anion to the hydrotalcite hydroxyl surface. (c) 2005 Elsevier B.V. All rights reserved.