Transcranial direct current stimulation (tDCS) may improve symptoms of inattention in adults with attention-deficit/hyperactivity disorder (ADHD). However, previous trials are characterized by small sample sizes, heterogeneous methodologies, and short treatment periods using clinic-based tDCS. To determine the efficacy and safety of home-based tDCS in treating inattention symptoms in adult patients with ADHD. Randomized, double-blind, parallel, sham-controlled clinical trial (tDCS for the Treatment of Inattention Symptoms in Adult Patients With ADHD [TUNED]), conducted from July 2019 through July 2021 in a single-center outpatient academic setting. Of 277 potential participants screened by phone, 150 were assessed for eligibility on site, and 64 were included. Participants were adults with ADHD, inattentive or combined subtype. Exclusion criteria included current stimulant drug treatment, current moderate to severe symptoms of depression or anxiety, diagnosis of bipolar disorder with a manic or depressive episode in the last year, diagnosis of schizophrenia or another psychotic disorder, and diagnosis of autism spectrum disorder; 55 of participants completed follow-up after 4 weeks. Thirty-minute daily sessions of home-based tDCS for 4 weeks, 2 mA anodal-right and cathodal-left prefrontal stimulation with 35-cm2 carbon electrodes. Inattentive scores in the clinician-administered version of the Adult ADHD Self-report Scale version 1.1 (CASRS-I). Included in this trial were 64 participants with ADHD (31 [48%] inattentive presentation and 33 [52%] combined presentation), with a mean (SD) age of 38.3 (9.6) years. Thirty participants (47%) were women and 34 (53%) were men. Fifty-five finished the trial. At week 4, the mean (SD) inattention score, as measured with CASRS-I, was 18.88 (5.79) in the active tDCS group and 23.63 (3.97) in the sham tDCS group. Linear mixed-effects models revealed a statistically significant treatment by time interaction for CASRS-I (βinteraction = -3.18; 95% CI, -4.60 to -1.75; P < .001), showing decreased symptoms of inattention in the active tDCS group over the 3 assessments compared to the sham tDCS group. Mild adverse events were more frequent in the active tDCS group, particularly skin redness, headache, and scalp burn. In this randomized clinical trial, daily treatment with a home-based tDCS device over 4 weeks improved attention in adult patients with ADHD who were not taking stimulant medication. Home-based tDCS could be a nonpharmacological alternative for patients with ADHD. ClinicalTrials.gov Identifier: NCT04003740.