Addiction is a psychiatric disorder characterized by loss of control over the consumption of psychotropic drugs despite adverse consequences. Nature has been a great source of metabolites of medicinal interest. Indeed, Nature has been a source of inspiration to scientists devoted to find pharmaceutics to treat drug addiction. Ibogaine, a natural tropane alkaloid, is one of the most natural products explored with respect to the antiaddiction properties. In this chapter, we primarily address the synthesis of ibogaine as well as its potential for the treatment of drug addiction. The antiaddiction properties of other natural products and related molecules are also discussed.