This article presents a history of the early electroencephalography (EEG) of psychopathy, delinquency, and immorality in Great Britain and the United States in the 1940s and 1950s. Then, EEG was a novel research tool that promised ground-breaking insights in psychiatry and criminology. Experts explored its potential regarding the diagnosis, classification, etiology, and treatment of unethical and unlawful persons. This line of research yielded tentative and inconsistent findings, which the experts attributed to methodological and theoretical shortcomings. Accordingly, the scientific community discussed the reliability, validity, and utility of EEG, and launched initiatives to calibrate and standardize the novel tool. The analysis shows that knowledge production, gauging of the research tool, and attempts to establish credibility for EEG in the study of immoral persons occurred simultaneously. The paper concludes with a reflection on the similarities between EEG and neuroimaging-the prime research tool in the current neuroscience of morality-and calls for a critical assessment of their potentials and limitations in the study of immorality and crime.