Objective: To evaluate the effect of iron on the attention deficit hyperactivity disorder, treated with methylphenidate. Methods: This double-blind, randomized placebo-controlled clinical trial was performed on 50 children with attention deficit hyperactivity disorder under the treatment of methylphenidate, with ferritin levels below 30 ng/ml and absence of anemia. They were randomly assigned into two groups of ferrous sulfate and placebo, for 12 weeks. Conners' Parent Rating Scale (CPRS) was used to assess the outcome in the first, sixth, and twelfth weeks. Results: Almost all CPRS subscales improved in the ferrous sulfate group from the baseline to the endpoint, although only the changes in conduct subscale scores were significant (p = 0.003). There was no significant difference in score changes between two groups in intergroup comparison. Also, the score of learning problems (p = 0.007) in the first six weeks, and conduct (p = 0.023) and psychosomatic (p = 0.018) subscales in the second six weeks were improved in the ferrous sulfate group compared with the placebo group. Conclusion Our study showed promising effects of iron supplementation in the improvement of subscales of the CPRS.