Magnesium and zinc titanium spinels are the white compounds with the basic formulas 2MgOTiO2 and 2ZnOTiO2, in which Mg2+ and Zn2+ can partly or wholly be replaced by other bivalent ions such as Co2+ and Ni2+. The ternary and the quarternary compounds thus obtained are coloured producing a great variety of hues.For the purpose of studying the properties of such pigments each constituents were mixed by dry process, calcined at the temperatures 1000°-1350°C. The reflectance between 400-750mμ were measured by a photo- electric spectrometer to represent the result by C. I. E. colour specification, and also X-ray analyses were made. The results are summarized as follows:(1) CoO-MgO-TiO2 system showed a wide variety of hues, ranging from light blue, through greenish blue, to medium and dark green. Pigments in this series had good brilliance, and the samples calcined at a temperature higher than 1200°C had the spinel structure.(2) NiO-MgO-TiO2 system gave no spinel structure in the samples heated at 1200°C, indicating that the formation of spinel was more difficult to occur than in the systems MgO-TiO2 and CoO-MgO-TiO2. The spinel structure was not found in NiOMgOTiO2 calcined at 1400°C, but NiOZnOTiO2 gave a light green pigment by calcining at 1200°C.(3) The spinel structure was not found in the system NiO-CoO-MgO-TiO2 when heated at 1200°C, but at 1350°C, and with increasing content of CoO, spinel was observed in the pigment whose colour changed from yellowish to brilliant green.(4) Pigments of the system CoO-ZnO-TiO2 gave colours ranging from light to dark yellowish brown, so that in NiO-CoO-ZnO-TiO2 series a clean brilliant hue could not be obtained with increasing amount of CoO.