Abstract Structured catalysts take advantage of high diffusion efficiency and low heat transfer resistance, effectively boosting reactions in non‐adiabatic gas–solid processes. However, traditional coating catalysts face problems of weak bond strength. Nanosized zeolites with rich hydroxyl as crystal seeds could effectively improve the binding strength of zeolite coatings, but their poor crystallinity resulted in low growth content. Here, we designed large‐size hollow zeolites and anatase as seeds to prepare metal@Silicalite‐1 structured catalysts. Hollow zeolites provided abundant nucleation sites and increased the growth content of zeolite by 1.8 times. Meanwhile, the abundant Si‐OH and the enriched surface Ti‐OH significantly strengthened the adhesion stability of the coatings. In the propane dehydrogenation reaction, the optimized PtZn@S‐1‐10HT exhibited a high specific activity of 14.1 mol C3H6 mol Pt −1 s −1 with propylene selectivity up to 96.4% at 600°C. This strategy breaks the inherent contradiction between high loading and strong binding ability of coating catalysts, which broadens the avenues for industrial applications.