This study described the development of a novel calcium ferrite/polyaniline nanocomposite, known as CaFe2O4-PANI nanocomposite, and investigated how well it would adsorb the hazardous anionic dye Eriochrome Black T (EBT). Results from XRD, SEM, FTIR, and BET characterizations verify the adsorbent's effective development. Brunauer-Emmett-Teller (BET) characterization method was applied to calculate the specific surface area and total pore volume of the fabricated CaFe2O4-PANI nanocomposite which were found to be 30.086 m2/g and 0.217 cc/g, respectively. The adsorbent shows enhanced EBT dye removal performance of approximately 90% at solution pH of 5.0, CaFe2O4-PANI dose of 1.0 g/L, contact time of 120 min and initial concentration of EBT dye 50 mg/L. The maximum uptake capability of 98.04 mg/g is achieved with the use of the Langmuir isotherm model and the adsorption method depicts best suitability for pseudo-second-order kinetic model. Additionally, the adsorbent was evaluated by introducing ions into dye samples and testing it against actual water samples. The results indicate a maximum drop in EBT dye removal effectiveness of approximately 10% and 32%, respectively, for wastewater samples and samples containing chloride ions. The experiment procedure had been improved using a five level and three factors based central composite design (CCD) with 20 test trials, and the generated quadratic model optimised maximal EBT elimination of 99.6%. Regeneration study implies less significant reduction in the dye extraction efficiency (~18%) even after 5 cycle of reuse of the adsorbent.