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This paper reports the formation of a solid solution in the system Bi2O3–TiO2–CuO. This solid solution seems to be isostructural with Bi4Ti3O12, according with the x-ray powder diffraction patterns. Microstructural studies done using scanning electron microscopy show the typical elongated Bi4Ti3O12 grain morphology only in samples with 2 : 2 : y molar ratios of the Bi2O3 : TiO2 : CuO oxides (y = 1, 2, or 3).