Objectives Vulnerable populations in underserved communities are disproportionately at high risk for multiple medical, dental, and behavioral health conditions. This study aims to: a) examine the occurrence of acute dental needs and b) investigate the association of acute dental needs and self-rated general and mental health status among the adult dentate health center population. Methods This cross-sectional study analyzed data on adult patients (n = 5,035) from the 2014 Health Center Patient Survey, a nationally representative survey of health center patients. Multivariate logistic regression was used to assess the association of acute dental needs and a) self-rated general health status and b) mental health status. Results Approximately, two thirds of adult dentate heath center patients reported having an acute dental need. After adjusting for confounding factors, not having or having had health insurance that pays for dental care, general health status of fair or poor, and ever having a mental illness were associated with higher odds of having an acute dental need. Conclusions The results highlight the role of health centers in addressing oral health disparities among vulnerable populations and the importance of a team-based multidisciplinary approach to ensuring the integration and coordination of oral health services within a comprehensive primary care delivery system.