Recently, there has been renewed interest in the potential use of psychoactive substances as pharmaceuticals. Like any other drug candidates, psychoactives also face a multitude of challenges in development for a diverse patient population. The crystal structure of a drug controls its important physical characteristics, significantly impacting drug properties like bioavailability. Recently, two older crystal creation technologies, polymorphism and cocrystallization, have reemerged to fabricate new and useful crystal forms for pharmaceuticals. To date, researchers in psychoactives have made only limited use of these novel techniques which therefore represent valuable technical opportunities for them.