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Light-emitting materials are of significant interest because of their vast potential applications in electroluminescent devices/displays and sensors. Herein, a novel bi-component supramolecular aggregation-induced emission (AIE) hydrogel (PDG) was successfully prepared with p-hydroxybenzonic acid-functionalized pillar[5]arene (SPA) and tri-(pyridine-4-yl)-functionalized trimesic amide (DTB) by a simple host–guest assembly process. The most attractive feature of PDG is its practical white-light-emitting property, which can be used for ultrasensitive detection and separation of Pb2+, Cr3+, and Fe3+ ions. The limits of lowest detection (LODs) of PDG for Pb2+, Cr3+, and Fe3+ are approximately 6.74 × 10−9, 7.18 × 10−9, and 8.25 × 10−9 M, respectively. Strikingly, by rationally introducing these metal ions into the PDG, a series of metal-ion-coordinated supramolecular metallogels PDG-Cr and PDG-Fe was constructed, and these metallogels can selectively detect CN− and H2PO4−, respectively. The LODs of PDG-Cr and PDG-Fe for CN− and H2PO4− reached up to 10−8 M. The prepared PDG-based thin films can act as a smart fluorescent display material and test kit. The xerogel of PDG can adsorb and separate Pb2+, Cr3+, and Fe3+ from aqueous solution, with adsorption rates ranging from 96.73% to 98.95%.