Multiple functional tailored materials have shown great potential for both pollutant degradation and freshwater recovery. In this study, we synthesized densely distributed Co onto carbon-layer-coated Ni/Al2O3 hydrangea composites (Ni/Al2O3@Co) via the polymerization of dopamine under a controlled graphitized process. The characterization results revealed that Ni/Al2O3@Co, with abundant exposed bimetallic Co-Ni species on the surface of Al2O3, could afford accessible catalytic sites for persulphate activation and subsequent pollutant degradation. The tetracycline (TC) degradation rate of optimal Ni/Al2O3@Co500 reached 98.1% within 15 min with a first-order rate constant of 0.498 min-1, which is ∼1.38 times that of Al2O3@Co500 (0.362 min-1), indicating the existing Co-Ni intermetallic synergy. Free radical quenching experiments indicated that ˙O2- plays a leading role in the catalytic degradation of TC. Moreover, Ni/Al2O3@Co500 afforded strong flexibility for the degradation of methylene blue (MB), norfloxacin (NFX), bisphenol A (BPA), and oxytetramycin (OTC). Ni/Al2O3@Co500 catalysts were anchored onto a customized sponge via a calcium-triggered hydrogel crosslink strategy to construct an integral and tailored stirrer, which was used directly as the mechanical stirrer catalyst for the activation of peroxymonosulfate and pollutant removal. This obtained stirrer was also used as a monolith evaporator affording an evaporation rate of 1.944 kg m-2 h-1 at a solar-driven photothermal interface. We also demonstrated that the shape of the tailored sponge weakly affects the course of the degradation reaction. Furthermore, the degradation rates of TC in actual water sources on a Ni/Al2O3@Co500 sponge were still maintained up to 90% with rational recycling properties, which provide a promising solution for the multiple-functional pollutant degradation and water regeneration.