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The pure and strontium (Sr) substituted LaFeO 3 polycrystalline samples were prepared through solid state synthesis process and good quality single crystals were successfully grown by four mirror optical floating zone technique for dielectric and magnetic measurements. The feed and seed rods were prepared by employing an external pressure of about 70 MPa and sintered at 1350 ⁰C on 12 h. The orthorhombic structure of the pure and Sr substituted materials were confirmed by powder X-ray diffraction analysis. The nonappearance of shoulder peaks in the Sr substituted LaFeO 3 sample reveals single-phase crystal system without any sub-grain boundaries. The composition of the pure and substituted crystals was confirmed by EDS (energy dispersive X-ray spectroscopy) analysis. The dielectric studies were carried out on both samples in the temperature range from 300 to 900 K for the frequency range from 2.5 kHz to 125 kHz. The grown crystals show their Neel temperature at 742 K and the dielectric constant value increased for substituted LaFeO 3 crystal. A colossal dielectric behavior and electrical conductivities were analyzed through dielectric studies. The activation energies of pure and Sr substituted LaFeO 3 crystals were estimated to be 0.19 and 0.16 eV respectively. Magnetic properties of the developed crystals were tested by M-H loop. The M-T plot of Sr substituted LaFeO 3 crystal was discussed with Zero field cooled (ZFC) and Field cooled (FC) modes for its potential magnetic application. • Peak shift of (121) plane confirms the lanthanide contraction in Sr substituted LaFeO 3 • At 742 K, Sr substituted LaFeO 3 crystal show enhanced dielectric constant, ɛ r = 3.25 × 105 • Ea value of LaFeO 3 and LaSrFeO 3 are 0.19 and 0.16 eV respectively • Sr substituted LaFeO 3 exhibits anti-ferro to ferromagnetic phase transition at 135 K • Sr substituted LaFeO 3 crystal shows improved coercivity, H c = 748.8164 Oe [ABSTRACT FROM AUTHOR]