The primary objective of this study is to elucidate the temperature-dependent polarization mechanisms of the diamond-like carbon (DLC) interlayered Schottky structures (SSs). The capacitance/conductance data were obtained for the temperature range of 80–410 K to achieve this objective, and the impedance spectroscopy method was utilized to ascertain the fundamental dielectric parameters, encompassing dielectric constant, dielectric loss, loss tangent, ac-conductivity, and electric modulus. Consequently, a significant behavioral disparity was observed by the parameters across three distinct temperature ranges, and these regions were classified as low (LTs), moderate (MTs), and high temperatures (HTs). The experimental findings have also demonstrated that various polarization mechanisms were either collectively or individually effective for the specific temperature regions. To elaborate further, it was understood that dipole polarization and trapping mechanisms were predominant in LTs, while Maxwell-Wagner mechanisms predominate in MTs. It has also been determined that space charge and Maxwell-Wagner polarizations were dominant mechanisms in HTs.