Reduced activity of the frontal lobes, and particularly of the prefrontal cortex, has been related with violent behavior, aggression and crime. The causal importance of prefrontal cortex activity for aggressive behaviors and the self-perception of aggressiveness needs however to be clarified. The aim of this study was to explore the effect of an anodal transcranial direct current stimulation protocol (tDCS, 1.5 mA, 15 min), which, according to previous studies, enhances cortical excitability, applied bilaterally over the prefrontal cortex on self-reported aggressiveness. Two imprisoned violent offender cohorts, discerned by the degree of aggressiveness (murderers vs. non-murderers), were included in this single-blind sham-controlled study. Self-reported aggressiveness was recorded before and after 3 tDCS sessions (one session per day). Four dimensions of aggression were evaluated by means of the standardized Buss-Perry Aggression Questionnaire (BAQ). In both inmate groups the results revealed an aggression-reducing effect of tDCS on the Physical aggression, Anger, and Verbal aggression dimensions of the BAQ. In the Hostility dimension, tDCS significantly reduced aggression only in the group of murderers. These results suggest that modulation of prefrontal cortex excitability by 3 consecutive sessions of tDCS reduces self-reported aggressiveness similarly in murderer and non-murderer samples.