Transcranial direct current stimulation (tDCS) is an emerging therapeutic tool for treating posttraumatic stress disorder (PTSD). Prior studies have shown that tDCS responses are highly individualized, thus necessitating the individualized optimization of treatment configurations. To date, an effective tool for predicting tDCS treatment outcomes in patients with PTSD has not yet been proposed. Therefore, we aimed to build and validate a tool for predicting tDCS treatment outcomes in patients with PTSD. Forty-eight patients with PTSD received 20 min of 2 mA tDCS stimulation in position of the anode over the F3 and cathode over the F4 region. Non-responders were defined as those with less than 50% improvement after reviewing clinical symptoms based on the Clinician-Administered DSM-5 PTSD Scale (before and after stimulation). Resting-state electroencephalograms were recorded for 3 min before and after stimulation. We extracted power spectral densities (PSDs) for five frequency bands. A support vector machine (SVM) model was used to predict responders and non-responders using PSDs obtained before stimulation. We investigated statistical differences in PSDs before and after stimulation and found statistically significant differences in the F8 channel in the theta band (p = 0.01). The SVM model had an area under the ROC curve (AUC) of 0.93 for predicting responders and non-responders using PSDs. To our knowledge, this study provides the first empirical evidence that PSDs can be useful biomarkers for predicting the tDCS treatment response, and that a machine learning model can provide robust prediction performance. Machine learning models based on PSDs can be useful for informing treatment decisions in tDCS treatment for patients with PTSD.