In the presence of inorganic salts, secondary organic aerosol (SOA) undergoes liquid-liquid phase separation (LLPS), liquid-solid phase separation, or a homogeneous phase in ambient air. In this study, a regression model was derived to predict aerosol phase separation relative humidity (SRH) for various organic and inorganic mixes. The model implemented organic physicochemical parameters (i.e., oxygen to carbon ratio, molecular weight, and hydrogen-bonding ability) and the parameters related to inorganic compositions (i.e., ammonium, sulfate, nitrate, and water). The aerosol phase data were observed using an optical microscope and also collected from the literature. The crystallization of aerosols at the effloresce RH (ERH) was semiempirically predicted with a neural network model. Overall, the greater SRH appeared for the organic compounds with the lower oxygen to carbon ratios or the greater molecular weight and the higher aerosol acidity or the larger fraction of inorganic nitrate led to the lower SRH. The resulting model has been demonstrated for three different chamber-generated SOA (originated from β-pinene, toluene, and 1,3,5-trimethylbenzene), which were internally mixed with the inorganic aqueous system of ammonium-sulfate-water. For all three SOA systems, both observations and model predictions showed LLPS at RH <80%. In the urban atmosphere, LLPS is likely a frequent occurrence for the typical anthropogenic SOA, which originates from aromatic and alkane hydrocarbon.