The immobilization of Hg 0 and detoxication of Hgcontaining composites are enormous challenges for Hg pollution control, which provide a high requirement for the design and synthesis of materials. Herein, a new composite with halloysite, selenium, and transition metals as raw materials (FeCo-LDH/ HNTs@Se) for a Hg 0 trap was designed by precipitation with ion exchange and an in situ selenization method. Intrinsic features such as high affinity, microwave permittivity (10 9 −10 12 ), large surface area, abundant pores, and many active components favored Hg 0 removal and immobilization. The removal performance, flue gas tolerance, and synergistic effect of active components were improved greatly when microwave was added. The study indicated that (1) the Hg 0 removal efficiency of the composite could reach 99.4%; (2) the composite had excellent tolerance to different industries' flue gases. The electron exchange of Co(II)/Co(III) and Fe(II)/Fe(III) and the existence of Se and SeO 2 were important for Hg 0 immobilization. HgSe was the main adsorption product based on both X-ray photoelectron spectroscopy (XPS) and an online lab-built thermal decomposition system (TPD-AFS) analysis, which made the used-materials possess low mercury leaching content (0.09 mg•L −1 ) lower than the US EPA regulatory value (0.2 mg•L −1 ). This work provides a sound way for mercury control, which is significant for environmental protection.