Building on eHealth literacy and mental health literacy, this cross-sectional survey study examined associations between eMental health literacy (the degree to which individuals obtain, process, and understand basic mental health information online to inform mental health-related decisions), perceived barriers to mental healthcare, and psychological distress. Data were collected online for 247 older adults in the United States. Higher eMental health literacy was associated with fewer perceived barriers to mental healthcare, in models conceptualizing psychological distress as an outcome of eMental health literacy and barriers to care (intrinsic, β = −0.36, p < .001; extrinsic, β = −0.24, p = .002) and as a covariate of eMental health literacy (intrinsic, β = −0.33, p = .001; extrinsic, β = −0.24, p = .003). Continued research and replication of findings are needed to better understand the potential role of eMental health literacy in reducing barriers to mental health services in later life.