Garnering support for smoke-free policies is critical for their successful adoption, particularly in countries with high smoking prevalence, such as Armenia and Georgia. In 2018, we surveyed 1456 residents (ages 18–64) of 28 cities in Armenia (n = 705) and Georgia (n = 751). We examined support for cigarette and electronic nicotine delivery systems (ENDS)/heated tobacco product (HTP) smoke-free policies in various locations and persuasiveness of pro- and anti-policy messaging. Participants were an average age of 43.35, 60.5% female, and 27.3% current smokers. Nonsmokers versus smokers indicated greater policy support for cigarette and ENDS/HTP and greater persuasiveness of pro-policy messaging. Armenians versus Georgians generally perceived pro- and anti-policy messaging more persuasive. In multilevel linear regression, sociodemographics (e.g., female) and tobacco use characteristics (e.g., smoking less frequently, higher quitting importance) correlated with more policy support. Greatest policy support was for healthcare, religious, government, and workplace settings; public transport; schools; and vehicles carrying children. Least policy support was for bar/restaurant outdoor areas. The most compelling pro-policy message focused on the right to clean air; the most compelling anti-policy message focused on using nonsmoking sections. Specific settings may present challenges for advancing smoke-free policies. Messaging focusing on individual rights to clean air and health may garner support.