Designing zeolites with tunable composition and acid siting is a significant challenge for applications in adsorption and catalysis. In their Communication on page 13366 ff., W. Chaikittisilp, J. D. Rimer, and co‐workers report on the synthesis of high‐silica faujasite (HOU‐3) with a Si/Al ratio of 3 and show that the Al locations within the structure are biased and not random. Cover designed by Koki Muraoka.