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This study examined differences in the associations between food insecurity and serious psychological distress (SPD) by key sociodemographic factors in a population-based sample of low-income adults from the 2017 California Health Interview Survey ( n = 6266). After adjusting for sociodemographic characteristics, low food security, and very low food security were both positively associated with SPD among all low-income adults. Upon stratification, these associations were most pronounced among adults under age 50, males, and in adults with children. Understanding disparities in the associations between food insecurity and psychological distress is critical in developing effective programs or policies to target the most vulnerable sub-groups.