The polycrystalline samples of GdFe1−xNixO3 (x = 0.0, 0.1, 0.2, 0.3) orthoferrites are synthesized via solid state reaction route. The Rietveld fitted X-ray diffraction patterns confirm the formation of orthorhombic phase with Pbnm space group for all the samples. The dielectric measurements reveal an enhancement in dielectric constant and tangent loss with increase in both temperature as well as Nickel (Ni) substitution. Dielectric studies are also in support with the induction of delocalized charge carriers in the GdFeO3 matrix with increasing Ni doping. Magnetization versus applied field study shows the non-saturating hysteresis curves suggesting the canted type antiferromagnetic behavior in the considered orthoferrites. Moreover, the observed magnetic behavior is complex and the doping affects the magnitude of magnetization differently at 300 K and 80 K. It has further been noticed that the incorporated Ni3+ ions enhances the symmetry of the magnetization curves. The as-prepared samples may find their applications in the decoupling capacitors.