Synthesis of lead tantalate pyrochlores by the reaction of PbO and Ta 2 O 5 in various molar ratios between 1.5 and 4.0 at low temperatures (500 -650°C) has been carried out. It has been shown that when PbO is reacted with Ta 2 O 5 in various molar ratios at low temperatures, metastable lead tantalate pyrochlore solid solutions having cubic symmetry are formed. X-ray diffraction data give evidence for an increase in the a lattice parameter with increasing PbO content and partial occupancy of Pb in the Ta sites leading to the formula Pb 1.5؉x 2؉ (Ta 2؊y Pb y 4؉ )O 7؊␦ (0.0 < x < 0.5; 0.0 < y < 0.6) for this phase. It has also been found that the intermediate members of the solid solutions are metastable and tend to segregate into Pb-deficient and Pb-excess compositions leading to significant compositional inhomogeneity for the intermediate members.