Accurate crystallization control is an essential aspect for chemical engineering and separation processes. Herein, we demonstrated the novelty of membrane crystallization (MCr) on the interfacial based‐crystal particle autoselection aimed for nucleation regulation and process control. With the proposed model based on a van der Waals‐friction‐hydrodynamic force field and classical nucleation theory, the motion mechanisms of heterogeneously induced nucleation were illustrated. The defined particle detachment criterion K revealed the control mechanism of the crystal particle motion behavior: temporary adherence, detachment, and perpetual adherence (scaling) at the membrane interface. For the first time, the function region of MCr (nucleation detection, scaling control, and crystallization regulation) was systematically illustrated and validated with the directly observed laboratory demonstration. These findings also demonstrate the potential applications of the uniform size distribution, morphology modified particle manufacture, and in situ nucleation detection. © 2018 American Institute of Chemical Engineers AIChE J, 65: 723–733, 2019