The present work explored the thermal properties, structure and crystallization kinetics of the anthracene (ANT)-carbazole (CAR) discontinuous binary solid solutions. The solid solutions with different stoichiometric ratios were synthesized by solid-state grinding or solution crystallization and characterized by differential scanning calorimetry and powder X-ray diffraction to explore their structure, morphology, and co-melting behavior. The molecular simulations results of the lattice energy of the constructed supercells also revealed the formation of ANT-CAR discontinuous solid solutions. The crystallization kinetics of the solid solutions were investigated, and the growth rate of the mixed crystals was determined using the population balance model.