A simple and convenient method for predicting critical constants (Tc, Pc, and Vc) for members of a homologous series was developed from computed molecular surface areas obtained from a molecular modeling program (CAChe version 3.5). The best linear correlations are obtained when Vc andTc /P0.5c are plotted against computed molecular surface area (SA) and when Tc and Pc are plotted against the natural logarithm of surface area, 1n SA, for 11 homologous series with a total of 118 organic compounds. The series included n-alkanes, n-alkyl primary amines, n-alkyl primary alcohols, acetate esters, n-alkyl primary thiols, secondary alcohols, n-alkylbenzenes, 2-methylalkanes, perfluoroalkanes, methyl esters, and ethyl esters. For C2-C19 n-alkanes, the calculated Tc (K) values agreed well with the literature critical temperatures (R = 1.000) and with other previously described correlations. Similar Tc correlations were found with the other 10 homologous series. The correlation between Tc/P0.5c and SA for the 11 homologous series is particularly striking and suggests a strong relationship between molecular surface area and intermolecular attractions.