A comparative study was performed to estimate biogas production from sludge produced by organic and inorganic chemically enhanced primary treatments (CEPTs). To this end, the effects of two coagulants, polyaluminum chloride (PACl) and Moringa oleifera (MO), on CEPT and biogas production in anaerobic digestion were surveyed within an incubation period of 24 days. The optimal dosage and pH of PACl and MO were optimized in terms of sCOD, TSS and VS parameters in the CEPT process. Next, the digestion performance of anaerobic digestion reactors fed with sludge obtained from PACl and MO coagulants at a batch mesophilic reactor (37 ± 1 °C) was surveyed from the biogas production, volatile solid reduction (VSR) and Gompertz model. At the optimal conditions (pH = 7 and dosage = 5 mg L-1), the removal efficiency of COD, TSS and VS in CEPT assisted with PACL was 63, 81 and 56%, respectively. Moreover, CEPT assisted with MO led to the removal efficiency of COD, TSS and VS until 55, 68 and 25%, respectively. The highest methane yield (0.598 L gVS removed-1) was obtained in an anaerobic digestion reactor with sludge from the MO coagulant. The anaerobic digestion of CEPT sludge instead of primary sludge resulted in higher sCOD removal efficiency, and 43-50% of sCOD was observed compared with the removal of 32% for the primary sludge. Furthermore, the high coefficient of determination (R2) demonstrated the trustworthy predictive precision of the modified Gompertz model with actual data. The combination of CEPT and anaerobic digestion, especially using natural coagulants, provides a cost-effective and practical way to increase BMP from primary sludge.