We report magnetoelectric coupling at room temperature between ferroelectric and magnetic order parameters in a Pb1xNixTiO3 (x=0.1, 0.3, and 0.5) system. These samples exhibited magnetism and ferroelectricity simultaneously at room temperature. The Ni substitution reduced the lattice distortion, i.e., ca ratio and, hence, the ferroelectric Curie temperature decreased. An anomaly in dielectric constant was observed in the vicinity of ferromagnetic Curie temperature. The magnetoelectric coupling at room temperature was evidence by the increase in saturation polarization after poling the samples in the magnetic field. For the Pb0.5Ni0.5TiO3 sample poled at 1.2 T of magnetic field, the increase in saturation polarization is about 11%.

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