Viscosity measurements of well-defined mixtures are useful in order to evaluate existing viscosity models. Recently, an extensive experimental study of the viscosity at pressures up to 140 MPa has been carried out for the binary systems methane + n-decane and methane toluene, between 293.15 and 373.15 and for several methane compositions. Although very far from real petroleum fluids, these mixtures are interesting in order to study the potential of extending various models to the simulation of complex fluids with asymmetrical components (light/heavy hydrocarbon). These data (575 data points) have been discussed in the framework of recent representative models (hard sphere scheme, friction theory, and free volume model) and with mixing laws and two empirical models (particularly the LBC model which is commonly used in petroleum engineering, and the self-referencing model). This comparative study shows that the average absolute deviation of the models is between 3.8 and 49.8%, and the maximum deviation is between 11.6 and 78.4%, depending on the considered model.