Sustained attention is defined as the ability to maintain attention over longer periods of time, which typically declines with time on task (i.e., the vigilance decrement). Previous studies have suggested an important role for the dorsomedial prefrontal cortex (mPFC) in sustained attention. In two experiments, we aimed to enhance sustained attention by applying transcranial electrical current stimulation over the mPFC during a sustained attention task. In the first experiment, we applied transcranial direct current stimulation (tDCS) in a between-subject design (n = 97): participants received either anodal, cathodal, or sham stimulation. Contrary to our prediction, we found no effect of stimulation on the vigilance decrement. In the second experiment, participants received theta and alpha transcranial alternating current stimulation (tACS) in two separate sessions (n = 47, within-subject design). Here, we found a frequency-dependent effect on the vigilance decrement, such that contrary to our expectation, participants’ performance over time became worse after theta compared with alpha stimulation. However, this result needs to be interpreted with caution given that this effect could be driven by differential side effects between the two stimulation frequencies. To conclude, across two studies, we were not able to reduce the vigilant decrement using tDCS or theta tACS.