This study examined contextually inappropriate (CI) anger in relation to emotion recognition and situation knowledge, negative social experiences, and externalizing behavior among low-income 4-year-olds attending Head Start (n = 134). Approximately 23% showed anger when presented with positive/neutral slides and videos (valence-incongruent CI anger), whereas 40% of children showed anger when presented with negative slides and videos (valence-congruent CI anger). Valence-incongruent CI anger was associated with lower emotion situation knowledge (for boys only), more self-reported peer rejection and loneliness, and greater negative nominations by teachers and peers. Both valence-incongruent and (for boys only) valence-congruent CI anger were positively associated with externalizing behavior. Overall, valence-incongruent CI anger was more strongly associated with negative child outcomes than valence-congruent CI anger.