Phosphorus pollution can induce water eutrophication and critically threaten the stability of the aquatic ecosystem. Capacitive deionization (CDI) is a potential candidate for controlling phosphorus levels due to its lack of chemical requirements, eco-friendliness, and low energy demand. Herein, a novel ZIF-67-derived CoAl-LDH embedded in conductive carbon skeletons (CoAl-LDH/C) was successfully constructed by a self-sacrificial template strategy. A conductive carbon matrix is incorporated into LDH, which can alleviate the insufficient conductivity and aggregation issues for LDH. The results revealed that CoAl-LDH/C possesses superior phosphorus elimination properties (qm=32.7 mg P/g) at 1.2 V, benefiting from its abundant active sites, large mesoporous diameter, specific surface area, total pore volume, outstanding specific capacitance, and ion diffusion. Meanwhile, the energy consumption of CoAl-LDH/C is merely 3.398 kWh/kg and 0.024 kWh/m3. CoAl-LDH/C also proved flexible for practical applications regarding complex water quality (wide pH range, coexisting substances, natural water) and cyclic utilization. Finally, the potential mechanism illuminated that the phosphorus elimination process in an electric field engages with ligand exchange, anion exchange, electrostatic attraction, and hydrogen bonds. This work paves a promising concept for designing innovative LDH-based electrodes with excellent ion diffusion and superior conductivity to eliminate phosphorus efficiently.