This study advanced knowledge on charisma by (a) introducing a new personality-based model to conceptualize and assess charisma and by (b) investigating curvilinear relationships between charismatic personality and leader effectiveness. Moreover, we delved deeper into this curvilinear association by (c) examining moderation by the leader’s level of adjustment and by (d) testing a process model through which the effects of charismatic personality on effectiveness are explained with a consideration of specific leader behaviors. Study 1 validated HDS charisma (Hogan Development Survey) as a useful trait-based measure of charisma. In Study 2 a sample of leaders (N = 306) were assessed in the context of a 360-degree development center. In line with the too-much-of-a-good-thing effect, an inverted U-shaped relationship between charismatic personality and observer-rated leader effectiveness was found, indicating that moderate levels are better than low or high levels of charisma. Study 3 (N = 287) replicated this curvilinear relationship and further illustrated the moderating role of leader adjustment, in such a way that the inflection point after which the effects of charisma turn negative occurs at higher levels of charisma when adjustment is high. Nonlinear mediation modeling further confirmed that strategic and operational leader behaviors fully mediate the curvilinear relationship. Leaders low on charisma are less effective because they lack strategic behavior; highly charismatic leaders are less effective because they lack operational behavior. In sum, this work provides insight into the dispositional nature of charisma and uncovers the processes through which and conditions under which leader charisma translates into (in)effectiveness.