The adsorption of carbon dioxide on hydrotalcite-like compounds was investigated. Two different powdered hydrotalcites were used containing the cations nickel and iron. The powdered materials were screened for carbon dioxide adsorption using a thermogravimetric method and it was found that NiMgAl (Sample 1) hydrotalcite has the largest capacity for CO2, adsorbing 1.58 mmol g(-1) at 20 degrees C, and highest rate of adsorption of up to 0.17 mmol g(-1) min(-1). This represented an increase of 53% in adsorption capacity, compared with NiMgAlFe (Sample 2). In order to improve the rheological behaviour of hydrotalcite paste for extrusion, hydrotalcite powders were combined with boehmite alumina (70:30 and 50:50 ratios of hydrotalcite:boehmite) before extrusion into pellets suitable for use in a fixed bed adsorber. These pellets were then re-crushed and further tested by thermogravimetric methods. The effects of temperature, composition and pre-treatment of the hydrotalcites on the adsorption of carbon dioxide and nitrogen are reported. At 20 degrees C, the amount of carbon dioxide adsorbed was between 2.0 and 2.5 mmol g(-1) for all the hydrotalcite/alumina samples in this study, although this decayed rapidly with increasing temperature. The results are compared with silica gel as a common sorbent reference, and with literature values. Hydrotalcite/alumina samples have thermal stability and a high adsorption capacity for carbon dioxide over a wide range of temperatures. The composition of the hydrotalcite/alumina pellets investigated in this study has less effect upon the adsorption behaviour compared with the non-calcined hydrotalcite powder, thus allowing a wide choice of pellet compositions to be used. (C) 2010 The Institution of Chemical Engineers. Published by Elsevier B.V. All rights reserved.