Y2FeAlO6 and YReFeAlO6 (Re = Nd, Sm, Gd, Dy) were successfully prepared by the solid-state reaction method. The crystal symmetry and stability are slightly improved under rare-earth substitution. The P-E ferroelectric hysteresis loops show that the YReFeAlO6 (Re = Nd, Sm, Dy, Gd) samples have weak room temperature ferroelectric properties with small remnant polarization (Pr = 0.0037–0.0168μC/cm2), which are slightly weaker than that of Y2FeAlO6 (Pr = 0.0367μC/cm2). The M-H hysteresis loops show that the magnetic properties of YReFeAlO6 (Re = Nd, Sm, Dy, Gd) are dominated by antiferromagnetic interaction, accompanied by weak ferromagnetism. The value of magneto-capacitance for YReFeAlO6 (Re = Nd, Sm, Dy, Gd) is higher than that of Y2FeAlO6, which indicates that the magneto-electric coupling enhances probably due to the decrease in the number of oxygen vacancies and the increase of the Fe3+ content under rare-earth substitution.