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Purpose: This study aimed to characterize the patterns of smoking, e-cigarette use, other substance use (alcohol and marijuana), and depression by sexual orientation in a sample of Mexican adult smokers. Methods: Data came from a 2018–2020 (six waves) online survey of adult smokers, recruited from a commercial research panel (92.5% heterosexual, n = 4786; 3.1% lesbian/gay, n = 160; and 4.4% bisexual, n = 229). After stratifying the data by sex, logistic, multinomial, and linear logistic regression models were estimated (depending on the outcome), including as independent variables sexual orientation (i.e., gay/lesbian, bisexual, heterosexual = Reference), age, education, household income, and wave. Results: Being a gay male was independently associated with greater smoking dependence (β = 0.20; 95% confidence interval [CI]: 0.02 to 0.39), greater likelihood of preference for flavored capsule cigarettes (adjusted odds ratio [AOR] = 2.10, 95% CI: 1.33 to 3.28), and depression diagnosis (AOR = 2.85, 95% CI: 1.64 to 4.95). Bisexual males had higher e-cigarette dependence (β = 0.37; 95% CI: 0.05 to 0.68, among dual users only) and were more likely to have been diagnosed with depression (AOR = 2.34, 95% CI: 1.30 to 4.18). Lesbian females were more likely to prefer menthol cigarettes (AOR = 3.32, 95% CI: 1.60 to 6.86), to have used marijuana more than once (AOR = 3.23, 95% CI: 1.83 to 5.72), and to have depressive symptoms (AOR = 1.85, 95% CI: 1.04 to 3.29). Bisexual females had a greater likelihood of depressive symptoms (AOR = 1.71, 95% CI: 1.14 to 2.56) and depression diagnosis (AOR = 2.22, 95% CI: 1.43 to 3.42). Conclusion: Lesbian, gay, and bisexual adult smokers in Mexico appear more likely than heterosexual adult smokers to report having depression. Substance use and depression among sexual minority populations need to be addressed further.