Anaerobic co-digestion of primary sludge with two types of drinking water treatment sludge (DWTS), namely iron- or aluminum-rich DWTS (Fe- or Al-DWTS) were systematically evaluated by biochemical methane potential tests, kinetic modelling, downstream process parameters and microbial community analysis. Specific methane yields decreased approximately 19% to 123 mL·g−1 VS, while the hydrolysis constant kh decreased from 0.21 d−1 to 0.18 d−1 for Fe-DWTS at 10% to 40% dosages. On the contrary, specific methane yields decreased 45–55% for Al-DWTS, and kh decreased to 0.14 d−1 at 40% dosage. Significant removals (>95%) of phosphate and hydrogen sulfide were observed for Fe- and Al-DWTS additions at 40% dosage. Microbial community analysis revealed that Al-DWTS increased the abundance of most hydrogenotrophic methanogens, while Fe-DWTS increased the abundance of acetoclastic methanogens. Kinetic modelling further revealed that Fe- and Al-DWTS additions affected the hydrolysis and methanogenesis process kinetics and the methane yield differently.