As previous studies have reported abnormalities in the iron indices of peripheral blood and hyperechogenicity of the substantia nigra (SN) in children and adolescents with attention-deficit/hyperactivity disorder (ADHD), we aimed to examine the same in adults with ADHD using transcranial Doppler sonography (TCS). In addition, we compared the iron indices and TCS findings before and after methylphenidate (MPH) treatment. A total of 39 participants aged ≥19 years (13 patients and 26 healthy controls) were recruited from Kyung Hee University Hospital between October 2018 and September 2019. All subjects were clinically evaluated based on the ADHD diagnostic criteria in the DSM-5, the Adult ADHD Self-Report Scale, and the Diagnostic Interview for ADHD in Adults (DIVA-5). Further, the iron indices including serum iron, ferritin, and mean platelet volume were determined. Additionally, TCS focused on the midbrain and echogenicity of the SN was conducted. Follow-up for all items was conducted for five ADHD patients after MPH treatment. Patients with ADHD had significantly lower education levels (number of years) than controls. There were no statistically significant differences in serum iron indices or the echogenic area between ADHD and control groups. Further, there were no significant changes in iron indices or TCS findings after MPH medication. Unlike previous studies, this study showed no differences between patients with ADHD and controls. Therefore, it is important to determine if these null findings were due to different target populations (children vs. adults) or other factors, including ADHD subtypes.