Background: Higher intakes of fruits and vegetables, rich in micronutrients, have been associated with better mental health. However, cooking or processing may reduce the availability of these important micronutrients. This study investigated the differential associations between intake of raw fruits and vegetables, compared to processed (cooked or canned) fruits and vegetables, and mental health in young adults.Methods: In a cross-sectional survey design, 422 young adults ages 18–25 (66.1% female) living in New Zealand and the United States completed an online survey that assessed typical consumption of raw vs. cooked/canned/processed fruits and vegetables, negative and positive mental health (depressive symptoms, anxiety, negative mood, positive mood, life satisfaction, and flourishing), and covariates (including socio-economic status, body mass index, sleep, physical activity, smoking, and alcohol use).Results: Controlling for covariates, raw fruit and vegetable intake (FVI) predicted reduced depressive symptoms and higher positive mood, life satisfaction, and flourishing; processed FVI only predicted higher positive mood. The top 10 raw foods related to better mental health were carrots, bananas, apples, dark leafy greens like spinach, grapefruit, lettuce, citrus fruits, fresh berries, cucumber, and kiwifruit.Conclusions: Raw FVI, but not processed FVI, significantly predicted higher mental health outcomes when controlling for the covariates. Applications include recommending the consumption of raw fruits and vegetables to maximize mental health benefits.