The promise of neurobiological interventions that afford improving pro-social behavior is particularly interesting for criminal justice systems. After all, rehabilitation of offenders is one of their central objectives. This raises the question of whether states can deploy such means to rehabilitate offenders against the latters’ will, as part of—or instead of—punishment. Some advocates of compulsory treatments of offenders consider them more humane (and effective) than current forms of hard treatment such as incarceration. This chapter critically engages with suggestions to treat legally competent offenders for rehabilitative purposes against their will by emphasizing two aspects. First, strong human rights of offenders—summarily the right to mental self-determination—oppose mandatory interventions into criminogenic psychological states or processes. These human rights are not (yet) recognized in every jurisdiction, but emerge from general liberal and democratic principles that most western jurisdictions endorse. Secondly, the case for mandatory rehabilitation is weaker than it may appear at first glance, because it is anything but clear that and why the penological aim of rehabilitation justifies severe interferences of offenders’ rights. In any case, it seems that states could attain their legitimate forward-looking aims—preventing recidivism—by less restrictive means such as incapacitation. Thus, compulsory rehabilitation may only be justified in exceptional cases. Rather, offenders should be offered a choice between neurorehabilitation and detention.