Background: Psychological well-being is associated with longevity and reduced risk of disease, but possible mechanisms are understudied. Health behaviors like eating fruits and vegetables may link psychological well-being with better health; however, most evidence is cross-sectional. Purpose: This study investigated psychological well-being’s longitudinal association with fruit and vegetable consumption across as many as 7 years. Method: Participants were 6,565 older adults from the English Longitudinal Study of Ageing, which includes men and women aged 50 years or older. Psychological well-being was assessed with 17 items from the Control, Autonomy, Satisfaction, Pleasure Scale. Fruit and vegetable consumption was initially assessed during 2006–2007 and then approximately every 2 years through 2012–2013. Covariates included sociodemographic factors, health status, and other health behaviors. Results: Mixed linear models showed that higher baseline levels of psychological well-being were associated with more fruit and vegetable consumption at baseline (β = 0.05, 95% confidence interval [CI] [0.02, 0.08]) and that fruit and vegetable consumption declined across time (β = −0.01, 95% CI [−0.02, −0.004]). Psychological well-being interacted significantly with time such that individuals with higher baseline psychological well-being had slower declines in fruit and vegetable consumption (β = 0.01, 95% CI [0.01, 0.02]). Among individuals who initially met recommendations to consume 5 or more servings of fruits and vegetables (N = 1,719), higher baseline psychological well-being was associated with 11% reduced risk of falling below recommended levels during follow-up (hazard ratio = 0.89, 95% CI [0.83, 0.95]). Conclusions: Findings suggest that psychological well-being may be a precursor to healthy behaviors such as eating a diet rich in fruits and vegetables. (PsycInfo Database Record (c) 2020 APA, all rights reserved