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In order to modulate the properties of LiTaO3 ceramics Li+ or Ta5+ cations have been substituted by mono-, di-, tri-, tetra-, penta- or hexavalent cations. A large number of solid solutions have been obtained, the observed nonstoichiometry corresponds either to a cationic excess or to a cationic deficit from LiTaO3. 7Li NMR measurements allowed the authors to point out the position of the substituted cations either in the tetrahedral or in the octahedral sites. The dependence of the Curie temperature T c vs composition has been determined. The variation of T c was related to width and intensity of the NMR quadrupole splitting.