A study of the Na 0.5 Bi 0.5 TiO 3 –PbTiO 3 and K 0.5 Bi 0.5 TiO 3 -PbTiO 3 systems has been carried out using X-ray diffraction, differential scanning calorimetry and dielectric measurements. The limits of the rhombohedral (Na 0.5 Bi 0.5 TiO 3 -rich side) and tetragonal (PbTiO 3 -rich side) solid solutions have been determined, as well as the evolution of their lattice parameters as a function of composition and temperature. Ceramic materials have been prepared by natural sintering (1090–1220 °C; 0.5 h) of powders obtained by solid-state reaction (900–1000 °C; 20 h) of the corresponding oxides and carbonates. The dielectric permittivities of these materials have been measured in a wide frequency range for temperatures between 20 and 800 °C. The results showed that they all are ferroelectric at room temperature and exhibit either a diffuse, probably second-order phase transition, or a sharp, first-order-like phase transition from the ferroelectric to the paraelectric state, depending on the composition.