• Room-temperature single phase multiferroic materials was obtained • Magnetoelectric coupling was observed at microwave (GHz) frequency • The coupling suggests a dynamic interaction between magnetic moments and ferroelectric polarization 0.63Bi 0.99 La 0.01 Fe 1- x Mn x O 3 -0.33BaTiO 3 -0.04Na 0.5 Bi 0.5 TiO 3 ( x = 0.10, 0.15, and 0.20) ceramics have been prepared by solid state reaction, and their structural, ferroelectric, ferromagnetic, piezoelectric, and magnetoelectric properties are studied. Except for the x = 0.2 composition, the X-ray diffraction and SEM-EDX analysis on the sintered ceramics show that the samples are single-phase, rhombohedral perovskites at room temperature. The introduction of Mn ions leads to a small deterioration in the ferroelectric and piezoelectric properties, whilst the room-temperature magnetization increases upon doping. The optimal multiferroic properties are obtained for the x = 0.15 composition. The magnetoelectric coupling in this sample was evidenced by the anomalies occurring simultaneously in the dielectric permittivity and magnetic permeability spectral profiles in the microwave region. Such a coupled phenomenon can be attributed to a dynamic interaction between magnetic moments and ferroelectric polarization.