Trait neuroticism predicts an increased risk of mortality. However, high levels of both neuroticism and conscientiousness (i.e., healthy neuroticism) are associated with various positive health behaviors. Eating behavior is a modifiable risk factor for obesity and metabolic diseases. This study investigated the cross-sectional and longitudinal associations between healthy neuroticism and eating behaviors. The data from the Nathan Kline Institute for Psychiatric Research-Rockland Sample included 712 adults with complete assessments of personality, eating behaviors, and metabolic markers. Linear and mixed linear regression models were used to examine cross-sectional and longitudinal associations of eating behaviors and personality traits, adjusting for sociodemographics, sleep quality, and body mass index (BMI). Healthy neuroticism cross-sectionally predicted the disinhibition and hunger dimensions of eating behavior, a result that withstood the inclusion of disease burden, clinical metabolic markers, and other personality traits. Longitudinally, healthy neuroticism did not predict changes in eating behavior. Greater conscientiousness scores were associated with increased restraint. These findings provide the first evidence that neuroticism is associated with less maladaptive eating behavior when modulated by conscientiousness. The implications of these associations for the relationships between eating behavior, metabolic health, and personality are discussed.