The study lowers the environmental risk by combining biodegradable adsorbents with stronger adsorption. This work uses two distinct kinds of adsorbents, namely Polyaniline (PANI) coated Kappa Cotton (KPC) and activated clay-biopolymer, Bentonite (aB) composite and Chitosan (CTN), to recover the aged transformer oil (aTO). Using the Box-Behnken (BB) design paired response surface method (RSM) approach, an experimental sequence was created to determine the optimal ratio of the adsorbent materials. The aTO was supplemented with the homogenized aB-CTN material (A*) and PANI-coated-KPC (B*) materials. After optimization, it was found that the optimal values for the input variables for the dielectric breakdown voltage and dielectric dissipation factor were A* = 1.76 g, B* = 1.28 g, temperature = 78.9 °C, while stirring duration = 3 h was kept constant. After treatment under ideal conditions, it was found that aTO1 had dielectric characteristics of 46.6 kV and 0.0020 dissipation factor, which are equivalent to those of laboratory studies conducted in triplicate with a 2.5 percent error. They demonstrate that aTO exhibits an outstanding dielectric response when the optimal proportion of the process variables (A* and B*) is used. The removal of impurities from aTO has considerably enhanced its dielectric properties, as seen by the CIE chromaticity coordinates, XRD analysis, UV responses, and FTIR analyses. The material’s ability to sorb dyes, polar impurities, and heavy metal ions is significantly increased by the expanded active sites of A* and B*.