The effect of thickness on distorted double perovskite structured BiFe0.5Cr0.5O3 (BFCO) thin films have been investigated for the first time using soft chemical method over Pt(111)/Ti/SiO2/Si substrate. The X‐ray diffraction (XRD) shows the presence of both BFO and BCO phases and confirms the formation of double perovskite‐structured BFCO. The morphology of the films changes with the increase in layers signifying the thickness dependence. The magnetization (M) versus magnetizing field (H) curve was well consistent with magnetoresistance (M‐R) results and exhibits anisotropic magnetoresistance. Thickness‐dependent dielectric behaviors of BFCO thin films were deeply understood from space charge, intrinsic and extrinsic mechanisms. The BiFe0.5Cr0.5O3 crystal systems with 60 nm thin layer showed an improved magnetism and magnetoresistance properties and are applicable to future magnetic application in the field of spintronics as a promising device.