The paper presents the development of a hybrid Monte Carlo (MC) method for the simulation of the simultaneous coagulation and phase segregation of an immiscible two-component binary aerosol. The model is intended to qualitatively model our prior studies of the synthesis of mixed metal oxides for which phase-segregated domains have been observed in molten nanodroplets. In our previous works (J. Aerosol Sci.32, 1479 (2001); Chem. Eng. Sci.56, 5763 (2001); submitted for publication) we developed sectional and monodisperse models where the internal state of the aerosol particles was described. These methods have certain limitations and it is difficult to include additional physical effects into the framework. Our new approach combines both constant volume and constant number Monte Carlo methods. Similar to our previous models, we assume that the phase segregation is kinetically controlled. The MC approach allows us to compute the mean number of enclosures (minor phase) per droplet, average enclosure volume, and the width of the enclosure size distribution. The results show that asymptotic behavior of enclosure distribution exists that is independent of initial conditions, which is very close to the continuum self-preserving distribution. Temperature is a key parameter because it allows for a significant change in the internal transport rate within each droplet. In particular, increasing the temperature significantly enhances the Brownian coagulation rate and lowers the number of enclosures per droplet. As a result, the MC results indicate that the growth of the minor phase can be moderated quite dramatically by small changes in system temperature. These results serve to illustrate the utility of this synthesis approach to the controlled growth of nanoparticles through the use of a majority matrix to slow down the encounter frequency of the minor phase and therefore its particle size.