The microstructure control and optimization of zeolite films and membranes is an indispensable challenge for various innovative applications. It can be steered by understanding the formation process. Here we design an unprecedented strategy to uncover direct evidence via the hydrothermal synthesis of chitosan-supported zeolite monolayers. The chitosan-supported layer involved in the hydrothermal reaction is observed using SEM, AFM, EPMA, and HRTEM while nucleation and crystal growth in the bulk synthesis solution are pursued with HRTEM, DLS, and SEM. The direct HRTEM observation is achieved on the chitosan-supported layer by peeling chitosan from its support. It reveals that a gel layer is initially formed on the chitosan layer where the subsequent crystal growth is fatally restrained. Our own experimental evidence and the literature reports clearly demonstrate that the formation mechanism is homogeneous for severely reduced crystal growth on the substrate but is heterogeneous when crystal growth on the substrate is significantly enhanced.