We reported the magnetic, dielectric and magnetoelectric properties of NdCrO3 polycrystalline ceramics. Magnetization curves revealed two magnetic transitions at 227 K and 38 K, which corresponded to Cr3+ canted antiferromagnetic ordering and Cr3+ spin reorientation phase transition, respectively. At 11.5 K, a Schottky-type anomaly was observed, caused by Nd3+ ground doublet Zeeman splitting. High-temperature dielectric relaxation exhibited a type of thermally activated relaxation process, which mainly resulted from the Maxwell–Wagner effect. The spin-reorientation of Cr3+ ions and the Nd3+ ground doublet splitting were observed to be accompanied by an electric polarization. The polarization could be induced by the presence of the antiferromagnetic-type domain walls, which led to spatial inversion symmetry breaking.