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Four-electron process and the interference of Cl- make sluggish kinetics on oxygen evolution reaction (OER) for seawater electrolysis. Herein, NiFe LDH grown on NiFe-foam with CeO 2 modification and (W 2 O 7)2- intercalation was synthesized by one-step hydrothermal method. It only needs 353.8 and 386.7 mV to achieve a large current density of 1000 mA·cm−2 in 1 M KOH and alkaline natural seawater, respectively. The catalytic material can stand 100 h with a retention of 98.1% at 1000 mA·cm−2 in alkaline natural seawater. Experiments and theoretical calculations confirm that the state-of-the-art OER activity comes from the introduced CeO 2 with optimized adsorption energy of intermediates. The improved stability and selectivity in seawater can be ascribed to the preferential adsorption of Ni and Fe with higher valence on OH- based on hard and soft acid based (HSAB) principle by (W 2 O 7)2- intercalation. This work provides a viable approach to develop efficient catalytic material for large-current seawater electrolysis. NiFe LDH nanosheets with (W 2 O 7)2- intercalation and CeO 2 modification show state-of-the-art large-current seawater-electrooxidation performance contributed partially from introduced CeO 2 adjusting adsorption energy of intermediates during OER process, partially from preferential adsorption of OH- on metal active sites based on hard and soft acid based (HSAB) principle by (W 2 O 7)2- intercalation. [Display omitted] • NiFe LDH nanosheets with (W 2 O 7)2- intercalation and CeO 2 modification have been successfully synthesized. • It only needs an overpotential of 386.7 mV to achieve 1000 mA cm−2 in alkaline natural seawater electrocatalysis. • (W 2 O 7)2- intercalation enhances OH- selectivity and CeO 2 modification optimizes adsorption energy towards OER intermediates. [ABSTRACT FROM AUTHOR]