Synthesis routes selective towards one framework usually rely on organic structure-directing agents (OSDAs) which template the pore and cage structure of the targeted material. However, selection of cost-effective OSDAs to crystallize the desired frameworks has historically depended on trial-and-error processes. While computational approaches have been developed to design OSDAs de novo, these methods often lead to complex OSDAs with low synthetic accessibility or low selectivity towards the targeted framework. Compared to pure-phase frameworks, intergrown zeolites exhibit a structure that is disordered in at least one dimension. Typically, intergrowths are formed by periodic building units related to each other by symmetry operations such as rotations or translations, 11 and whose stacking enables them to form a defect-free interface between two topologically distinct domains. Although manually describing such structural faults is possible, 11 computational methods have enabled enumerating intergrown families such as ABC-6 12 or simulating diffraction patterns. More recently, structural descriptors have been proposed to quantify whether two phases are topologically or geometrically compatible to form intergrown structures. As differences in local crystallographic environments affect confinement and transport properties, intergrowth zeolites display catalytic behavior distinct from the pure end-member phases. For example, the silicoaluminophosphate form of the CHA/AEI intergrowth is a competitive catalyst for the methanol-to-olefin (MTO) reaction compared to the commercial SAPO-34 catalyst. 17,18 However, the challenges of selective zeolite synthesis are exacerbated in the case of intergrowths. Traditional routes for synthesizing the high-silica form of CHA/AEI require the combination of two specific OSDAs for CHA and AEI, which increases the synthesis complexity and cost. In addition, tuning the synthesis conditions to favor the formation of the desired intergrowth requires labor-intensive experimentation.