Unraveling the mechanism of zeolite crystallization, especially in a complex system containing dual-template agents, remains a critical challenge. In this work, we introduced, for the first time, novel operando two-dimensional (2D) solid-state NMR spectroscopy under extreme conditions of high temperature and high pressure, allowing for observations with atomic-level spatial and temporal resolution, thereby enabling unprecedented insights into the crystallization of SAPO-34 zeolite. By utilizing operando 2D