The highly toxic and recalcitrant organic pollutant, 2,4-dichlorophenol (2,4-DCP), is commonly found in wastewater. Therefore, it is critical to investigate novel techniques for the efficient removal of 2,4-DCP from wastewater. The present study employed a one-step synthesis method to fabricate ZIF-8/multi-walled carbon nanotubes (ZIF-8/MWCNTs) nanocomposites with well-defined mesoporous structures, which were subsequently coated onto carbon cloth (CC) to form the anode ZIF-8/MWCNTs/CC. Subsequently, the adsorption performance of ZIF-8/MWCNTs toward 2,4-DCP and the adsorption-electrochemical degradation performance of ZIF-8/MWCNTs/CC toward 2,4-DCP were investigated. ZIF-8/MWCNTs exhibit exceptional adsorption capacity and rate toward the 2,4-DCP. At 303 K, it achieved a saturated adsorption amount as high as 1056.78 mg·g−1 within only 30 min of reaching equilibrium. Moreover, when coated on CC substrates, the internal pore structure of ZIF-8/MWCNTs is effectively exploited during the adsorption. In addition, the incorporation of MWCNTs enhances the conductivity of the ZIF-8/MWCNTs/CC electrodes, leading to reduced resistance and improved electron transfer rate. Notably, ZIF-8/MWCNTs/CC enabled complete removal of a 25 mg·L-1 solution of 2,4-DCP within only 90 min and a 50 mg · L-1 solution within 120 min. Furthermore, the degradation mechanism of 2,4-DCP was analyzed by means of DFT modeling theoretical calculations and intermediate product determination analysis, while evaluating the toxicity of the generated material was evaluated. This study provides improved solutions and strategies for the treatment of chlorophenolic compound pollution in wastewater.