Homeless persons experience a high burden of health problems; yet, they face significant barriers in accessing health care. Less is known about unmet needs for care among vulnerably housed persons who live in poor-quality or temporary housing and are at high risk of becoming homeless. The objectives of this study were to examine the prevalence of and factors associated with unmet needs for health care in a population-based sample of homeless and vulnerably housed adults in three major cities within a universal health insurance system. <i>Methods</i> Participants were recruited at shelters, meal programs, community health centers, drop-in centers, rooming houses, and single room occupancy hotels in Vancouver, Toronto, and Ottawa, Canada, throughout 2009. Baseline interviews elicited demographic characteristics, health status, and barriers to health care. Logistic regression was used to identify factors associated with self-reported unmet needs for health care in the past 12 months. <i>Results</i> Of the 1,181 participants included in the analysis, 445 (37%) reported unmet needs. In adjusted analyses, factors associated with a greater odds of reporting unmet needs were having employment in the past 12 months (AOR = 1.40, 95% CI = 1.03–1.91) and having >=3 chronic health conditions (AOR = 2.17, 95% CI = 1.24–3.79). Having higher health-related quality of life (AOR = 0.21, 95% CI = 0.09–0.53), improved mental (AOR = 0.97, 95% CI = 0.96–0.98) or physical health (AOR = 0.98, 95% CI = 0.96–0.99), and having a primary care provider (AOR = 0.63, 95% CI = 0.46–0.85) decreased the odds of reporting unmet needs. <i>Conclusions</i> Homeless and vulnerably housed adults have a similar likelihood of experiencing unmet health care needs. Strategies to improve access to primary care and reduce barriers to accessing care in these populations are needed.