We have explored the possibility of ferromagnetic semiconducting property in the epitaxial thin films of LaFe 1−x Ni x O 3 ͑x = 0.3, 0.4, and 0.5͒ grown on ͑001͒ oriented LaAlO 3 substrate. We observe that substitution of Ni in the series leads to the increase in conductivity of the samples with conduction being controlled by the disorder-induced localization of charge carriers. All these samples show ferromagnetic behavior at room temperature while their magnetization decreases with increase in Ni concentration in the composition. The results have been explained on the basis of the close interplay between the electrical and magnetic properties. © 2005 American Institute of Physics. ͓DOI: 10.1063/1.2058218͔Over the last few years, there has been extensive study in the direction of search for the materials possessing ferromagnetic property as well as the semiconducting property because of their potential applications in the spintronics devices, wherein the spin-controlled electrical, optical, and magnetic properties are desired. 1,2 The study has yielded several systems such as magnetic multilayers, 3 Fe 3 O 4 , 4 perovskite-based transition metal oxides etc. 5 Study of transition metal oxides ͑TMOs͒, has revealed an impressive diversity of exciting physical properties such as dielectric, magnetic, optical, and transport properties because of the strong electron correlation effect in the system. The TMOs exhibit high-T c superconductivity in cuprate systems; metalinsulator ͑MI͒ transition, colossal magnetoresistance, and charge ordering in manganites; and many other phenomena in other TMO systems. [5][6][7][8] Among several TMO-based systems of LaTO 3 ͑T = Fe, Co, Cr, Ni, and Mn͒, LaNiO 3 has rhombohedral perovskite structure and is a Pauli-paramagnetic metal with high electrical conductivity at room temperature, 9 while the other TMO systems are generally antiferromagnetic insulators, except for LaFeO 3 , which shows ferrimagnetic transition at Néel temperature T N ϳ 750 K. 10-14 Therefore, the series of LaNi 1−x Fe x O 3 samples provides an ideal opportunity to observe an interesting co-occurrence of MI transition accompanied with a paramagnetic to ferrimagnetic transition in the same member of the series at a critical substitution concentration of Fe/ Ni ions. This presents a prospect to investigate the Mott's criterion of the dependence of MI transition on the critical charge carrier density by examining in such series from its one end member ͑LaNiO 3 ͒ to the one at the other end ͑LaFeO 3 ͒.There are several reports available on bulk samples of LaNi 1−x Fe x O 3 series by various groups including ours, where disorder-induced MI transition, structural transition from rhombohedral ͑LaNiO 3 ͒ to orthorhombic ͑LaFeO 3 ͒ at Fe concentration of ϳ50%, and the inverse dependence of itinerancy of d electrons with the Fe concentration have been observed. [15][16][17][18] It is suggested that in these systems the MI transition is due to the potential mismatch between the substituent metal ion and Ni +3 ion, which cause...