Introduction: E-cigarette use has surged during the past few years while the debate about the product's safety and efficacy for smoking cessation continues. Little is known about the characteristics that distinguish users from nonusers; in this study, we aimed to elucidate these characteristics among hospitalized smokers, a heretofore unstudied population. Methods: Cross-sectional data were collected from cigarette smokers via hospital bedside interviews. Participants reported e-cigarette use status, reasons for use (if used), e-cigarette advertising exposure, expected likelihood of future e-cigarette use, desire to quit smoking, and demographic characteristics. Results: Of the 657 English-speaking hospitalized smokers who provided data, 97% reported awareness of e-cigarettes and 46.4% reported e-cigarette use, with 20% reporting use in the previous 30 days. Previous e-cigarette use was significantly more likely among those who were White (odds ratio [OR] = 4.7; confidence interval [CI] = 3.2-6.7), were married/had a domestic partner (OR = 1.5; CI = 1.0-2.2), had more than a high school education (OR = 1.7; CI = 1.1-2.7), had e-cigarette advertising exposure (OR = 1.6; CI = 1.1-2.4), and were younger (OR = 1.3; CI = 1.1-1.5). Expected likelihood of future e-cigarette use was high and positively correlated with desire to quit smoking (Spearman's ρ = .18, p < .0001). Conclusions: Rates of awareness and use of e-cigarettes may be elevated among hospitalized smokers, with more use reported among those who were White, younger, more educated, in a relationship, and exposed to e-cigarette advertising. The association between desire to quit smoking and expected likelihood of future e-cigarette use suggests that cigarette smokers may perceive e-cigarettes as a useful cessation aid.