Two optimization approaches to correct the physical limitations of the Lee–Kesler–Plöcker equation of state for the application to long-chain hydrocarbons are presented. The quality of the approaches is evaluated by comparisons with experimental data and reference equations of state. The calculation of thermodynamic properties for alkanes up to squalane is possible with both approaches, for some of which no highly accurate fundamental equation of state is available in the literature. For the first approach, the original parameter set was refitted with constraints guaranteeing correct behavior of the equation in the liquid state. The densities of long-chain hydrocarbons are reproduced with small deviations, while the results for some short-chain alkanes are worsened. For the second approach, existing Helmholtz energy equations of state are utilized, while keeping the linear interpolation scheme via the acentric factor. Significant improvements are achieved for all fluids considered.