Despite the rapid rise in the number of blended education studies after the COVID-19 pandemic, the topics of self-regulated and mobile-mediated learning in blended tertiary education environments is an open research issue. The purpose of this pilot study is to identify tertiary education students’ perceived enablers/facilitators and barriers to self-regulated and mobile-mediated learning in blended education environments. Nineteen undergraduate and postgraduate students were interviewed in Greece, and data were analyzed through descriptive analysis. According to the findings, most participants believed that blended learning helps their autonomy and self-regulated learning when they are facilitated by ownership of, ease of use, and familiarity with mobile devices. Major enablers/facilitators, but also barriers to, self-regulated and mobile-mediated learning in blended contexts are the course structure (mainly, the online component of blended education, appropriateness of learning activities, and educational material), and individual (educators’ knowledge, skills, confidence, and attitudes, and students’ knowledge, skills, and concerns) and technological (infrastructure and internet connectivity) factors. Students’ expectations concerning blended education courses are associated with the course organization (e.g., provision of alternative learning possibilities, balance between face-to-face and digital/online learning activities, and access to various teaching material/tools) and the role of students and teachers. Implications for students, educators and university policy and practice are discussed.