Layered　double　hydroxide　(LDH)　catalysts　provide　promising　OER　activity　which　can　be　employed　in　overall　water　splitting　for　hydrogen　production.　However,　their　weak　surface　hydrogen　adsorption　(Had)　and　high　water　dissociation　energy　can　result　in　the　inferior　hydrogen　evolution　reactions　(HER)　activity.　In　this　paper,　a　highly　efficient　HER　catalyst　of　F-doped　NiCoMo　LDH　is　successfully　designed　and　synthesized　through　in　situ　growing　on　nickel　foam　(F-NiCoMo　LDH/NF)　for　overall　water　splitting.　DFT　calculations　demonstrate　that　the　introduction　of　Mo　and　F　atoms　in　NiCo　LDH　can　induce　the　generation　of　anisotropic　lattice　strain,　resulting　in　the　generation　of　high-energy　active　interface　and　shifting　the　d-band　centers.　Therefore,　the　adsorption　energy　of　Had　is　optimized　and　the　water　dissociation　energy　barrier　is　decreased.　As　a　result,　this　F-NiCoMo　LDH/NF　catalyst　electrode　displays　a　low　overpotential　of　107.5　mV　at　10　mA　cm−2　and　a　small　Tafel　slope　of　67.2　mV　dec−1　for　HER.　The　assembled　electrolyzer　by　employing　this　catalyst　electrode　requires　only　1.83　V　to　deliver　300　mA　cm−2　and　operates　stably　for　100　h.　©　2023　The　Electrochemical　Society　(“ECS”).　Published　on　behalf　of　ECS　by　IOP　Publishing　Limited.