Objective: Caffeine and dietary supplement (DS) use by college students is not well-documented. Given reported associations between energy drink consumption and sensation seeking, we used the Sensation Seeking Scale Form V (SSS-V) to assess relationships between sensation-seeking, caffeine, and DS use. Participants: Data from 1,248 college students from five US institutions were collected from 2009 to 2011. Methods: Linear regression was used to examine relationships between scores on the SSS-V and caffeine and DS use, demographic, and lifestyle characteristics. Results: Male sex, nonHispanic race-ethnicity, higher family income, tobacco use, consuming caffeinated beverages, more than 400 mg caffeine per day, and energy drinks with alcohol at least 50% of the time, were significantly associated with higher total SSS-V scores (P < 0.001). Those using protein DSs had higher total, disinhibition, and boredom susceptibility SSS-V scores (Ps < 0.001). Conclusions: Results demonstrate a positive correlation between sensation-seeking attitudes and habitual caffeine, energy drink, and DS consumption.