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In this paper, a random-forest-based method was proposed for the classification and localization of Attention-Deficit/Hyperactivity Disorder (ADHD), a common neurodevelopmental disorder among children. Experimental data were magnetic resonance imaging (MRI) from the public case-control dataset of 3D images for ADHD-200. Each MRI image was a 3D-tensor of 121 × 145 × 121 size. All 3D matrices (MRI) were segmented into the slices from each of three orthogonal directions. Each slice from the same position of the same direction in the training set was converted into a vector, and all these vectors were composed into a designed matrix to train the random forest classification algorithm; then, the well-trained RF classifier was exploited to give a prediction label in correspondence direction and position. Diagnosis and location results can be obtained upon the intersection of these three prediction matrices. The performance of our proposed method was illustrated on the dataset from New York University (NYU), Kennedy Krieger Institute (KKI) and full datasets; the results show that the proposed methods can archive more accuracy identification in discrimination of ADHD, and can be extended to the other practices of diagnosis. Moreover, another suspected region was found at the first time. [ABSTRACT FROM AUTHOR]