Ferric iron is widely dosed in wastewater treatment plants dealing with sulfide for septicity control, which generates a great amount of iron-rich chemical sludge that is challenging and costly to dispose. This study investigates the feasibility of using this iron sludge as the electron donor for autotrophic denitrification, not only realizing high nitrogen removal efficiency without additional carbon source requirement, but also partially mitigating iron-rich chemical sludge disposal and reduce sludge production by enriching low-yield autotrophic denitrifiers in the system. Both batch tests and performance monitoring of a lab-scale up-flow anaerobic sludge blanket reactor with a more than 300 days of operation were conducted. All the results confirmed the feasibility of using iron sludge as electron donor for autotrophic denitrification. The nitrate reduction rate with iron sludge was highly influenced by the type of ferrous electron donor and the electron donor/acceptor ratio. Ferrous hydroxide had significantly higher nitrate reduction rate than ferrous sulfide at the same electron donor/acceptor ratio. The nitrate reduction rate also accelerated with the increase of the electron donor/acceptor ratio. However, if the total surface area of the iron sludge is considered for comparison, it was shown that ferrous hydroxide and ferrous sulfide provided similar nitrate reduction rates of around 0.02 mmol N/m2/d in this study, indicating total surface area would be the key parameter for denitrification efficiency for the solid phase electron donor.