This study employed latent growth curve analysis to evaluate the interactive effects of two specific facets of impulsivity (i.e., negative urgency [NU] and premeditation [PRE]) and negative emotions (NE) on the developmental trajectory of nonsuicidal self-injury (NSSI) among 3,453 (57% females) Chinese community adolescents. Participants completed questionnaires assessing NSSI, NU, PRE, and NE (i.e., depression, anxiety, and stress) at three waves of time. The initial levels of NE and NU significantly predicted the initial level of NSSI. Changes in NE and NU significantly predicted change in NSSI. Moreover, the initial levels of NU and PRE significantly moderated the relationship between the initial levels of NE and NSSI, such that among individuals with higher NU or less PRE, the three NE were associated with a higher level of NSSI. Additionally, among individuals with a faster increase in NU, depression and anxiety were associated with a faster increase in NSSI. These findings suggest that adolescents with trait impulsivity, especially in the form of NU, are more vulnerable to the engagement in NSSI.