Which post‐synthetic modification strategy is the best suited for the generation of particular textural or chemical features in mordenite for a desired catalytic application? The aim of this contribution is to shed light on the effective quality of zeolite hierarchization through the rational study of structure/catalytic property dependency. Our study focused on mordenite, as this zeolite is of particular importance due to its strong acidity and monodimensional channel system, which explains why mordenite is industrially extensively employed. A toolbox of post‐synthetic hierarchization strategies on aluminum rich and poor mordenites has been developed based on basic treatments assisted by CTAB and pyridine at various temperatures (in conventional and microwave heating) and acid HF etching in aqueous and organic medium. A systematic study of over 30 post‐synthetically modified mordenites was conducted, which allowed us to assess the impact of each hierarchization strategy on textural, morphological, chemical and catalytic properties. Major correlations between structural features and catalytic activity, selectivity and stability in both the monomolecular n‐hexane cracking and the bimolecular toluene disproportionation were deduced.