Emotion regulation difficulties are present in many, if not most, children with attention-deficit/hyperactivity disorder (ADHD) and confer risk for a host of adverse outcomes. Little is known, however, regarding the neurocognitive and behavioral mechanisms that underlie these difficulties. A well-characterized, clinically evaluated sample of 145 children ages 8–13 years (M = 10.33, SD = 1.47; 55 girls; 69% White/non-Hispanic) were administered multiple, counterbalanced working memory tests and assessed for emotion dysregulation and ADHD symptoms via multiple-informant reports. Bias-corrected, bootstrapped conditional effects modeling indicated that underdeveloped working memory exerted significant direct effects on emotion regulation in all tested models as well as indirect effects on emotion regulation via parent-reported hyperactive/impulsive symptoms (95% CIs excluded zero). Interestingly, hyperactive/impulsive symptoms also predicted emotion dysregulation when controlling for the influence of working memory. Inattention failed to predict emotion regulation difficulties in all tested models (all 95% CIs included zero). This pattern of results replicated across parent and teacher models and were robust to control for mono-informant bias, age, and gender. These findings suggest that emotion dysregulation in ADHD reflects, in part, both a direct outcome of underdeveloped working memory and an affective outcome of hyperactive and/or impulsive symptomatology, both attributable to and independent of the role of underlying working memory deficits.