ABSTRACT Achieving controlled synthesis of silicoaluminophosphate (SAPO) zeolites is critical for optimizing their catalytic performances, yet it remains difficult due to the complex coupling of synthesis variables and insufficient atomic‐level structural understanding. Herein, we systematically investigate the multi‐scale characterization and controllable synthesis of SAPO zeolites. We explore the effects of critical synthesis parameters (pH, Si content, the concentration and composition ratio