Supramolecular polymers have attracted increasing attention in recent years due to their perfect combination of supramolecular chemistry and traditional polymer chemistry. The design and synthesis of macrocycles have driven the rapid development of supramolecular chemistry and polymer science. Pillarnarenes, a new generation of macrocyclic compounds possessing unique pillar‐shaped structures, nano‐sized cavities, multi‐functionalized groups, and excellent host–guest complexation abilities, are promising candidates to construct supramolecular polymer materials with enhanced properties and functionalities. This review summarizes recent progress in the design and synthesis of pillararene‐based supramolecular polymers (PSPs) and illustrates their diverse applications as adsorption and separation materials. All performances are evaluated and analyzed in terms of efficiency, selectivity, and recyclability. Typically, PSPs can be categorized into three typical types according to their topologies, including linear, cross‐linked, and hybrid structures. The advances made in the area of functional supramolecular polymeric adsorbents formed by new pillararene derivatives are also described in detail. Finally, the remaining challenges and future perspectives of PSPs for separation‐based materials science are discussed. This review will inspire researchers in different fields and stimulate creative designs of supramolecular polymeric materials based on pillararenes and other macrocycles for effective adsorption and separation of a variety of targets. Supramolecular polymer materials have attracted significant attention for wide potential applications in numerous fields, particularly in adsorption and separation, due to the elegant combination of supramolecular chemistry with polymer science. This review highlights the recent advancements in pillararene‐based supramolecular polymers for adsorption and separation applications, with an emphasis on their synthetic strategies, adsorption mechanisms, and separation performances.