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Optimized Pt/WO3–ZrO2 catalysts were evaluated in the isomerization of C5–C6 paraffins. The catalysts were tailored for optimal activity and selectivity using both the model C6 paraffin mixtures and C5–C6 real raw feeds from the industrial production of high quality gasoline. The optimization included a study of the role of the structure of Pt/WO3–ZrO2 undoped and doped with aluminum, with focus on the nuclearity and nature of WO3 species. The heterogeneity of the structure, acid and redox properties were analysed using UV–Vis and Raman, and supplemented by temperature programmed reduction with hydrogen and desorption of ammonia. The results show a maximum achieved increment of R.O.N. = 14, using a mixture of hexane isomers (hexane g.r.) as raw material, which demonstrated the potential of these materials for an environmentally friendly process for the improvement of transportation fuels.