In this work, we extend the previously reported study of global phase diagrams in binary mixtures relevant for the description of natural gases using the perturbed-chain statistical associating fluid theory (PC-SAFT) model to systems containing n-alkanes + other nonlinear hydrocarbons. These mixtures have branched, cyclic, and aromatic compounds and provide a deeper insight into the effect upon their thermodynamic behavior by introducing additional structural complexity into the mixtures. The studied systems show different patterns of phase equilibria according to the van Konynenburg classification. The PC-SAFT model usually describes properly the previously reported n-alkane + n-alkane binary mixtures, including their varied and complex phase behavior. The results reported in this work contribute to a better understanding of the binary mixtures fluid-phase behavior and show the ability of the PC-SAFT model to describe the thermodynamic properties of these systems and to model complex intermolecular effects, and they can be useful for the modeling and understanding of natural gas properties in industrial applications.