AbstractAn extensive critical evaluation of available correlations for predicting critical properties of binary defined hydrocarbon as well as some multicomponent hydrocarbon and hydrocarbon‐nonhydrocarbon mixtures is presented using all available literature data. The Li method is recommended for critical temperature prediction based upon its accuracy and simplicity, although the Chueh‐Prausnitz method is equivalent in accuracy. The Kreglewski method is most accurate for critical pressure prediction. All methods evaluated yielded high errors for the critical properties of methane‐containing mixtures. Current correlations on critical volume are discussed, and correlational work on prediction using an excess volume approach is described.