The structural, magnetic, and electrical properties of new series La0.5Nd0.5Cr1-xFexO3 (x = 0.0, 0.2, 0.4, 0.6, 0.8, 1.0) have been reported. All the phases crystallize in the orthorhombic symmetry with Pbnm space group. The unit cell volume of La0.5Nd0.5Cr1-xFexO3 increases monotonically with increasing Fe doping. Magnetization studies showed that all our investigated phases (except x = 0.8 and 1.0) exhibit a paramagnetic–anti-ferromagnetic transition at low temperature. The variation in Neel temperature (TN) with increasing x can be explained in terms of magnetic interactions due to Fe doping. Irreversibility between the zero-field-cooled (ZFC) and field-cooled (FC) magnetization is clearly seen close to TN. All the phases show that insulating behavior and the transport properties are dominated by the polaron hopping mechanism with increase in polaron hopping energy with Fe content.