
Precise control of the framework configuration in crystalline materials is a pivotal theme in materials science. The characteristics of zeolites are critically dependent on the Al siting in their frameworks. Although numerous synthesis-based strategies have been sought to regulate Al siting in specific zeolites, a universally applicable and more precise methodology remains in high demand. Here, we propose a postsynthetic approach to manipulate Al siting. This proposed hydrothermal treatment effectively modified Al siting in MAZ-type zeolites without altering their overall composition or structure. A combined experimental and computational analysis revealed the achievement of an optimal atomic configuration around extra-framework cations. This strategy opens up a new avenue for controlling Al siting, thereby enhancing the functional performance of the zeolites.