University students (N543) watched film clips to manipulate negative, neutral, or positive mood states and then performed a mood regulation task with the goal of experiencing positive affect. Autonomic reactivity was assessed during habituation, mood inductions, and mood regulation. According to the mood-behavior model (G.H.E. Gendolla, 2000) and studies on self-regulation, we predicted stronger cardiovascular and electrodermal reactivity in a negative mood than in both positive and neutral moods in the context of mood regulation but not during the mood inductions. Results were as expected. Furthermore, the Zygomaticus Major muscle reacted more strongly in the positive than in the neutral and negative mood conditions during the mood inductions. The findings are interpreted as demonstrating mood effects on resource mobilization during an effortful mood regulation performance.