In this work, single-phase nanostructured NdFe1−xCoxO3 (x = 0, 0.1, 0.2, and 0.3) perovskite materials were obtained by annealing stoichiochemistry mixtures of their component hydroxides at 750 °C for 60 min. The partial substitution of Fe by Co in the NdFeO3 crystal lattice leads to significant changes in the structural characteristics, and as a consequence, also alters both the magnetic and optical properties of the resulting perovskites. The low optical band gap (Eg = 2.06 ÷ 1.46 eV) and high coercivity (Hc = 136.76 ÷ 416.06 Oe) give Co-doped NdFeO3 nanoparticles a huge advantage for application in both photocatalysis and hard magnetic devices.