The Framework Convention on Tobacco Control mandates the creation of smoke-free environments to protect non-smokers from second-hand smoke and reduce demand for tobacco. We aimed to examine the extent and nature of smoke-free campus policies at tertiary education institutions throughout New Zealand, and examine the policy development process. Stage one comprised an audit and content analysis of smoke-free policies. In stage two, semi-structured telephone interviews were conducted to investigate the process of developing and implementing policies. Qualitative content analysis was undertaken on interview notes. Policies were identified for most institutions (n = 26/29), though varied widely in nature. Only nine mandated 100% smoke-free campuses without exceptions and few prohibited the sale of tobacco on campus, or connections with the tobacco industry. During interviews (n = 22/29), cited barriers to developing a 100% smoke-free policy included enforcement challenges and anticipated opposition from staff and students. However, participants from institutions with 100% smoke-free policies reported having encountered few challenges. Varying levels of compliance with 100% smoke-free policies were reported yet, overall, these policies were viewed as being effective. Smoke-free campus policies could be strengthened to better reflect a completely tobacco-free organization. Other institutions and workplaces could use these findings to develop 100% smoke-free policies.