Crystal violet (CV) dye, because of its non-biodegradability and harmful effects, poses a significant challenge for wastewater treatment. This study addresses the efficiency of easily accessible coal fly ash (CFA)-based adsorbents such as raw coal fly ash (RCFA) and surface enhanced coal fly ash (SECFA), in removing CV dye from waste effluents. Various analytical techniques such as FTIR, XRD, SEM, TEM, BET, zeta sizer and zeta potential were employed for the characterization of the adsorbents and dye-loaded samples. BET revealed that RCFA possesses a surface area of 19.370 m2 g-1 and SECFA of 27.391 m2 g-1, exhibiting pore volumes of 0.1365 cm3 g-1 and 0.1919 cm3 g-1 respectively. Zeta-sizer and potential analysis showed the static charges of RCFA as -27.3 mV and SECFA as -28.2 mV, with average particle sizes of 346.6 and 315.3 nm, respectively. Langmuir and Freundlich adsorption isotherms were also employed for adsorption studies. Employing central composite design (CCD) of response surface methodology (RSM), the maximum CV removal was 81.52% for RCFA and 97.52% for SECFA, providing one minute contact time, 0.0125 g adsorbent dose and 10 ppm dye concentration. From the thermodynamic studies, all the negative values of ΔG° showed that all the adsorption processes of both adsorbents were spontaneous in nature.