Frontal alpha asymmetry (FAA) is a neural correlate of approach and avoidance motivational processes. This study examined the shift in FAA from baseline to play, associations to parent-reported regulatory abilities, and parent and infant behaviors during play. Infants exhibited greater left frontal alpha activity (more approach) during baseline relative to play. Shifts in FAA toward greater left frontal alpha activity (more approach) from baseline to play were associated with parent ratings of infants' regulatory behaviors and object exploration exhibited during play. These results highlight ongoing regulatory processes involved in positively valenced tasks typical in infants' daily life.