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Homelessness is a priority public health issue in the United States (U.S.) given its strong associations with multiple adverse health outcomes. While overall rates of homelessness have decreased over the last decade, some populations—such as sexual and gender minorities—have not seen equitable decreases. The present study explores the relationship between experiences of first-time homelessness with substance misuse (assessed via the DAST-10) and depression and anxiety (assessed via the PHQ-4) in an adult sample of SGM individuals in South Central Texas. The analytic sample (n = 907) was majority gay/lesbian or same-gender loving (55.8%) followed by bisexual or pansexual (34.7%) or another sexual identity (9.5%) and 12.5% were transgender. First-time homelessness was more common in childhood than adulthood. Multivariate logistic regression models were used to evaluate relationships between first-time homelessness and outcomes of interest. The odds of substance misuse (DAST > 3) were marginally higher for those experiencing first-time homelessness in childhood and significantly higher for those reporting first-time homelessness in adulthood. The odds of experiencing past 2-week depression were significantly greater for those reporting homelessness in childhood or adulthood. However, only first-time homelessness in adulthood was significantly associated with past two-week anxiety. These findings underscore the need to consider intersectionality when exploring solutions to existing health disparities, as this work suggests that both sexual and gender identity and homelessness are important factors in shaping mental and behavioral health outcomes. [ABSTRACT FROM AUTHOR]