Self-stabilized precipitation (2SP) polymerization provides a new way for the high-value utilization of substantial olefin fractions in the petrochemical industry. However, the fundamental mechanism of particle nucleation and growth remains poorly understood. In this work, we present a general picture of 2SP polymerization, and the nucleation process is modeled by a dynamic population balance equation. The nucleation period involves primary particle aggregation and reduction in the particle number density prior to the emergence of a colloidally stable steady-state particle number density in 2SP polymerization. The model simulations exhibited reasonable agreement with the experimental conversion, particle diameter, and particle number density over the course of the reaction. This investigation not only advances the understanding of 2SP polymerization but also contributes insights into the broader realm of heterogeneous polymerization mechanisms.