Background: U.S. adults experience challenges in performing and sustaining healthy behaviors to improve their cardiovascular health. Self-monitoring modalities may facilitate these lifestyle changes. Therefore, the objective of this cross-sectional study was to examine the use of self-monitoring modalities and the association between the use of multiple self-monitoring modalities and participants’ population characteristics, health behaviors, and status. Methods: Data were drawn for the Health Information National Trends Survey 5, Cycle 1. The study included 3,285 U.S. adults, 18 years or older. Descriptive statistics examined the use of different types of self-monitoring modalities. Binary and ordered logistic regression analyses examined the relationship between the types of self-monitoring modalities and participants’ population characteristics, health behaviors, and status. Tableau Software was used to illustrate study results. Results: The average age of participants was 54.3 years. Smartphone/tablet users were more likely to have completed college (45.28%) compared to electronic monitoring device users (41.06%) and online medical record users (34.04%). Among smartphone/ tablet users, participants had significantly higher odds of consuming >4 cups of fruits/ vegetables than ≤4 cups of fruits/vegetables [odds ratio (OR) = 2.27, 95 confidence interval (CI) = 1.32–3.90]. An increase in the number of self-monitoring modalities used was associated with a higher odds of participants consuming >4 cups of fruits/vegetables compared to participants who consumed <4 cups of fruits/vegetables (OR = 1.76, 95% CI = 1.13–2.76). Conclusions: Findings of this study highlight that U.S. adults are utilizing a variety of modalities to monitor their health. Several self-monitoring modalities were associated with consuming the recommended amount of fruits/vegetables and performing moderate physical activity for >150 minutes/week. Further research is warranted to understand how to utilize population characteristics, health behavior, and status to promote the efficacy of self-monitoring.