Moral systems universally prohibit harming others for personal gain. However, we know little about how such principles guide moral behavior. Using a task that assesses the financial cost participants ascribe to harming others versus themselves, we probed the relationship between moral behavior and neural representations of profit and pain. Most participants displayed moral preferences, placing a higher cost on harming others than themselves. Moral preferences correlated with neural responses to profit, where participants with stronger moral preferences had lower dorsal striatal responses to profit gained from harming others. Lateral prefrontal cortex encoded profit gained from harming others, but not self, and tracked the blameworthiness of harmful choices. Moral decisions also modulated functional connectivity between lateral prefrontal cortex and the profit-sensitive region of dorsal striatum. The findings suggest moral behavior in our task is linked to a neural devaluation of reward realized by a prefrontal modulation of striatal value representations.