Due to their nanoporous framework structures, zeolites have been widely used as catalysts, adsorbents, and ion exchangers in many industrial fields. Discovering zeolitic materials with new structures and desired functions is one of the most important tasks in the zeolite community. Traditional zeolite discovery relies primarily on low-efficiency trial-and-error processes. So far, many computational and experimental efforts have been devoted to the designed synthesis of zeolitic materials, representing a promising highway toward function-led discovery of nanoporous materials. In particular, the design of structure-directing agents, the design of target zeolites via structure enumeration, and the reorganization of disassembled building layers have led to the discovery of dozens of unprecedented zeolitic structures in the past 5 years. In this Perspective, we briefly discuss these advances and describe the research efforts that are needed in the coming era of function-led zeolite discovery.