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　(H-ad)　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　H-ad　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.