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Background: There is a lack of consensus in the literature about the association between the perceived health risks of e-cigarettes and their actual use, an association that may be based on cigarette smoking status or sexual and gender minority status. This study examined the moderating effect of these variables as well as differences in e-cigarette use between and within perceived harmfulness of e-cigarettes and cigarette smoking among U.S. adults. Methods: The data were drawn from the 2020 and 2019 Health Information National Trends Survey (HINTS 5), Cycles 4 and 3, on adults (N= 9303). We estimated weighted multivariable logistic regression models and conducted marginal analyses based on perceived harmfulness of e-cigarettes. Results: Of the study population, 30.75% currently used e-cigarettes daily or some days. No significant difference in e-cigarette use was found between sexual minorities and heterosexuals, but there was a significant interaction between sexual identity and perceived harmfulness of e-cigarettes. Compared to non-smokers, current daily or some days cigarette smokers were more likely to use e-cigarettes (AOR = 3.48, 95% CI = 1.25, 9.72). Those who perceived e-cigarettes to be just as harmful as actual cigarettes (AOR = 0.13, 95% CI = 0.06, 0.27) or more harmful (AOR = 0.03, 95% CI = 0.01, 0.10), or were uncertain (AOR = 0.18, 95% CI = 0.08, 0.45), were less likely to use e-cigarettes compared to those who perceived e-cigarettes to be less harmful. Former and current cigarette smokers who perceived e-cigarettes as less harmful had a higher probability of using e-cigarettes daily or some days than did non-cigarette smokers. For the current and former cigarette smoking groups, those who perceived e-cigarettes as less harmful had the highest probability of current e-cigarette use than did those who were uncertain or perceived e-cigarettes as just as harmful, whereas the probability was not significant for those who perceived e-cigarettes as more harmful. Conclusion: Current daily or some days use of e-cigarettes is associated with current daily or some days cigarette smoking and lowered perceived harmfulness of e-cigarettes among the U.S. adult population. Tailored health promotion and intervention efforts may reduce the potential perceived health and behavioral/lifestyle risks related to the use of tobacco products, especially the use of e-cigarettes daily among former and current cigarette smokers as well as those who perceive e-cigarettes as less harmful.