Fifteen equimolar binary mixtures are synthesized and thermophysically evaluated in this study. These mixtures are derived from six ionic liquids (ILs) based on methylimidazolium and 2,3-dimethylimidazolium cations with butyl chains. The objective is to compare and elucidate the impact of small structural changes on the thermal properties. The preliminary results are compared to previously obtained results with mixtures containing longer eight-carbon chains. The study demonstrates that certain mixtures exhibit an increase in their heat capacity. Additionally, due to their higher densities, these mixtures achieve a thermal storage density equivalent to that of mixtures with longer chains. Moreover, their thermal storage density surpasses that of some conventional materials commonly used for energy storage.