The present study compares the treatment of pharmaceutical industry wastewater (PIWW) by coagulation‐flocculation (C‐F) and electrocoagulation (EC) techniques using response surface methodology (RSM). EC was performed with waste food‐grade Aluminium (Al) foil as a sacrificial anode. In C‐F, to minimize chemical usage, dual coagulants Aloe vera (organic) and ferric chloride (chemical) were used. Optimization using RSM for C‐F showed chemical oxygen demand (COD) reduction of 60.25 ± 0.28% at optimum operating conditions with R2 = 0.964 and adj‐R2 = 0.928, whereas EC resulted in COD reduction of 78.23 ± 0.38% and energy consumption 1.498 ± 0.0076kWh/m3 with R2 = 0.978 and adj‐R2 = 0.956. The result showed that the use of food‐grade waste Al foil as anode electrode (in EC) and the use of dual coagulant (in C‐F) can reduce COD from industrial effluent efficiently contributing to less hazardous sludge generation.