[Display omitted] • Self-assembled monolayers (SAMs) with different groups were prepared on a gold quartz monitor crystal. • SAMs played dominant role on the selectivity of polymorphism during crystallization of carbamazepine. • Piezoelectric effect of quartz monitor crystal makes that SAMs induced crystallization can be in-situ monitored. • The metastable zone of carbamazepine with different forms induced by different SAMs were established. • SAMs modified gold quartz monitor crystal can realize two requirements simultaneously: selection of polymorphism and in-situ monitoring of crystallization. Compared with traditional control methods in the drug crystallization process, a heterogeneous functional monolayer is an effective approach that could induce needed crystal forms under easier control conditions. In this study, a QCM sensor modified by functional groups was used to control the CBZ polymorphism, analyze the process of SAM formation and demonstrate the crystallization process of template-induced heterogeneous nucleation. The results showed that the heterogeneous functional monolayer reduced the induction time of the crystallization and controlled the polymorphism of pharmaceutical crystals. At the same time, molecular modeling was also applied to study the crystallization growth mechanisms of CBZ on the SAM. This work provides a reliable and promising new idea for the controlled crystallization of more drug systems and the online analysis of the nucleation process, and also provides a precise new means for the exploration of the crystallization mechanism. [ABSTRACT FROM AUTHOR]