This study explored the association between number of methods of Nonsuicidal Self-Injury (NSSI) and personality, psychopathology, and functions of NSSI. Two combined undergraduate samples reporting a history of NSSI (n = 149) completed measures of personality, psychopathology, and NSSI. A series of regression analyses indicated that Conscientiousness, Openness, and two functions of NSSI (i.e., Automatic Negative Reinforcement and Social Negative Reinforcement) shared significant relationships with the number of NSSI methods participants engaged in. These findings demonstrate that, after accounting for NSSI frequency, a relationship exists among specific personality factors, NSSI functions, and engagement in additional methods of NSSI.