Nanocrystalline mordenite (MOR) zeolites were hydrothermally synthesized in a single step with commercial cetyltrimethylammonium (CTA) hydroxide as the sole organic template, while the aluminum source was varied in a typical synthesis gel. CTA can effectively reduce the crystal growth of MOR zeolites, in some cases selectively in the a‐ and b‐directions of the unit cell. These nanocrystalline MOR zeolites do not only have a larger external surface area than their bulk counterparts prepared without CTA, but the Brønsted acid sites in the side‐pockets are also more accessible. The combination of the use of CTA and AlCl3 ⋅ 6H2O afforded the best‐performing catalyst with much improved activity in benzene alkylation and hydroconversion of n‐hexadecane (n‐C16). Modifying MOR synthesis with CTA hydroxide is a cheap and effective method to open up the one‐dimensional micropore system of mordenite, increasing the catalytic performance in hydrocarbon reactions.