Background Young adults (18–25 years) are struggling with the transition to becoming autonomous users of healthcare services. Although barriers to healthcare accessibility for young adults, such as service cost and difficulty navigating the healthcare system, have been identified, the interactions and relationships between these barriers have not been explored in depth. Methods A narrative literature review was conducted to determine the foundational knowledge and communication skills needed by young adults to effectively interact with the healthcare system. Semi-structured interviews were conducted with young adults from New South Wales and the Australian Capital Territory Australia to explore their experiences of healthcare and barriers to their care, and the potential for education based on the identified necessary knowledge and skills to improve their experiences. Results Inductive thematic analysis of 11 interviews showed young adults’ experiences of barriers across policy, institutional, community, interpersonal, and individual levels. These factors contributed to suboptimal healthcare experiences and impeded participants’ ability to effectively communicate with healthcare providers, leading to eroding trust between providers and young adult patients. All participants supported the subsequent recommendations of education priorities for young adults, expecting increased confidence and ability to self-advocate if provided teaching based on the suggested content. Conclusions This paper highlights specific targets and directions for future health policy and health education initiatives to improve the healthcare experiences of young adults.