Exposure therapy is highly effective for anxiety-related disorders, but there is a need for enhancement. Recent trials of adjunctive neuromodulation have shown promise, warranting evaluation of transcranial direct current stimulation (tDCS) as an augmentation. In a double-blind, placebo-controlled trial, contamination- and animal-phobic participants (N = 49) were randomized to active tDCS (1.7 mA, 20 min; n = 27), or sham tDCS (1.7 mA, 30 s; n = 22), followed by 30 min of in-vivo exposure. Active tDCS targeted excitation of the left mPFC and inhibition of the right dlPFC; polarity was counterbalanced for controls. We predicted tDCS would result in accelerated and better maintained gains, contingent on the subsequent in-session response, and baseline negative prognostic indicators. Consistent with predictions, tDCS promoted engagement and reductions in threat appraisals during exposure, and greater reductions in distress and threat appraisals through 1-month, although effects did not uniformly generalize. tDCS was most beneficial given high phobic severity, anxiety sensitivity, and a suboptimal early response. tDCS may promote engagement and response among individuals who are resistant or refractory to standard treatment. tDCS should be applied to more severe anxiety-related disorders, with parameters yoked to individual differences to improve outcomes in exposure-based interventions.