Despite the United States having one of the leading health care systems in the world, underserved minority communities face significant access challenges. These communities can benefit from telehealth innovations that promise to improve health care access and, consequently, health outcomes. However, little is known about the attitudes toward telehealth in these communities, an essential first step toward effective adoption and use. The purpose of this study is to assess the factors that shape behavioral intention to use telehealth services in underserved Hispanic communities along the Texas-Mexico border and examine the role of electronic health (eHealth) literacy in telehealth use intention. We used cross-sectional design to collect data at a community health event along the Texas-Mexico border. The area is characterized by high poverty rates, low educational attainment, and health care access challenges. Trained bilingual students conducted 322 in-person interviews over a 1-week period. The survey instrument assessed sociodemographic information and telehealth-related variables. Attitudes toward telehealth were measured by asking participants to indicate their level of agreement with 9 statements reflecting different aspects of telehealth use. For eHealth literacy, we used the eHealth Literacy Scale (eHEALS), an 8-item scale designed to measure consumer confidence in finding, evaluating, and acting upon eHealth information. To assess the intention to use telehealth, we asked participants about the likelihood that they would use telehealth services if offered by a health care provider. We analyzed data using univariate, multivariate, and mediation statistical models. Participants were primarily Hispanic (310/319, 97.2%) and female (261/322, 81.1%), with an average age of 43 years. Almost three-quarters (219/298) reported annual household incomes below $20,000. Health-wise, 42.2% (136/322) self-rated their health as fair or poor, and 79.7% (255/320) were uninsured. The overwhelming majority (289/319, 90.6%) had never heard of telehealth. Once we defined the term, participants exhibited positive attitudes toward telehealth, and 78.9% (254/322) reported being somewhat likely or very likely to use telehealth services if offered by a health care provider. Based on multivariate proportional odds regression analysis, a 1-point increase in telehealth attitudes reduced the odds of lower versus higher response in the intention to use telehealth services by 23% (OR 0.77, 95% CI 0.73-0.81). Mediation analysis revealed that telehealth attitudes fully mediated the association between eHealth literacy and intention to use telehealth services. For a 1-point increase in eHEALS, the odds of lower telehealth use decreased by a factor of 0.95 (5%; OR 0.95, 95% CI 0.93-0.98; P<.001) via the increase in the score of telehealth attitudes. Telehealth promises to address many of the access challenges facing ethnic and racial minorities, rural communities, and low-income populations. Findings underscore the importance of raising awareness of telehealth and promoting eHealth literacy as a key step in fostering positive attitudes toward telehealth and furthering interest in its use.