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Background: Adults with mental illnesses are more likely to have low income and diet-related chronic diseases., Objective: This study examined associations of mental illness diagnosis status with food insecurity and diet quality and whether the relationship between food security status and diet quality differed by mental illness diagnosis status in adult Medicaid beneficiaries., Design: This was a secondary cross-sectional analysis of baseline (2019-2020) data collected as part of the LiveWell study, a longitudinal study evaluating a Medicaid food and housing program., Participants/setting: Participants were 846 adult Medicaid beneficiaries from an eastern Massachusetts health system., Main Outcome Measures: Food security was measured with the 10-item US Adult Food Security survey module (0 = high food security, 1-2 = marginal food security, 3-10 = low/very low food security). Mental illness diagnoses included health record-documented anxiety, depression, or serious mental illness (eg, schizophrenia, bipolar disorder). Healthy Eating Index (HEI-2015) scores were calculated from 24-hour dietary recalls., Statistical Analyses: Multivariable regression analyses adjusted for demographics, income, and survey date., Results: Participants' mean (standard deviation) age was 43.1 (11.3) years, and 75% were female, 54% Hispanic, 33% non-Hispanic White, and 9% non-Hispanic Black. Fewer than half (43%) of participants reported high food security, with almost one third (32%) reporting low or very low food security. The 341 (40%) participants with one or more mental illness diagnosis had greater odds of low/very low food security (adjusted odds ratio [OR], 1.94; 95% confidence interval [CI], 1.38-2.70) and had similar mean HEI-2015 scores (53.1 vs 56.0; P = 0.12) compared with participants with no mental illness diagnosis. Mean adjusted HEI-2015 scores did not significantly differ by high vs low/very low food security for those without a mental illness diagnosis (57.9 vs 54.9; P = 0.052) or those with a mental illness diagnosis (53.0 vs 52.9; P = 0.99)., Conclusion: In a cohort of adults with Medicaid, those with mental illness diagnoses had higher odds of experiencing food insecurity. Overall, diet quality among adults in this sample was low but did not differ by mental illness diagnosis or food security status. These results highlight the importance of augmenting efforts to improve both food security and diet quality among all Medicaid participants., (Copyright © 2023 Academy of Nutrition and Dietetics. Published by Elsevier Inc. All rights reserved.)