The present study is focused on the procedure of spray- and freeze-drying techniques for the preparation of Cr-doped sphene pigments (CaSn0.98Cr0.02SiO5, CaTi0.98Cr0.02SiO5) from an aqueous solution of precursor salts, followed by calcinations of the resulting powders in absence of additives. The evolution of the present crystalline phases with applied thermal treatments was studied by X-ray powder diffraction and thermal analysis. The powder morphology was analysed by scanning electronic microscopy. The behaviour of the chromium ion was clarified by ultraviolet and visible spectroscopy. The colour efficiency of pigments was evaluated by colourimetric analysis (CIE L*a*b* system). (C) 2009 Elsevier B.V. All rights reserved.