Cognition and emotion, traditionally thought of as largely distinct, have recently begun to be conceptualized as dynamically linked processes that interact to influence functioning. This study investigated the moderating effects of cognitive functioning on the relationship between negative emotionality and attention deficit/hyperactivity disorder (ADHD) symptom severity. A total of 216 (140 hyperactive/inattentive; 76 typically developing) preschoolers aged 3–4 years were administered a neuropsychological test battery (i.e., NEPSY). To avoid method bias, child negative emotionality was rated by teachers (Temperament Assessment Battery for Children-Revised), and parents rated symptom severity on the ADHD Rating Scale (ADHD-RS-IV). Hierarchical Linear Regression analyses revealed that both negative emotionality and Perceptual-Motor & Executive Functions accounted for significant unique variance in ADHD symptom severity. Significant interactions indicated that when negative emotionality is low, but not high, neuropsychological functioning accounts for significant variability in ADHD symptoms, with lower functioning predicting more symptoms. Emotional and neuropsychological functioning, both individually and in combination, play a significant role in the expression of ADHD symptom severity. (JINS, 2011, 17, 502–510)