We present a dataset combining human-participant high-density electroencephalography (EEG) with physiological and continuous behavioral metrics during transcranial electrical stimulation (tES). Data include within participant application of nine High-Definition tES (HD-tES) types, targeting three cortical regions (frontal, motor, parietal) with three stimulation waveforms (DC, 5 Hz, 30 Hz); more than 783 total stimulation trials over 62 sessions with EEG, physiological (ECG, EOG), and continuous behavioral vigilance/alertness metrics. Experiment 1 and 2 consisted of participants performing a continuous vigilance/alertness task over three 70-minute and two 70.5-minute sessions, respectively. Demographic data were collected, as well as self-reported wellness questionnaires before and after each session. Participants received all 9 stimulation types in Experiment 1, with each session including three stimulation types, with 4 trials per type. Participants received two stimulation types in Experiment 2, with 20 trials of a given stimulation type per session. Within-participant reliability was tested by repeating select sessions. This unique dataset supports a range of hypothesis testing including interactions of tDCS/tACS location and frequency, brain-state, physiology, fatigue, and cognitive performance.