The interfacial water has recently been identified as an important factor that influence the kinetics of HOR/HER. Yet there is a debate on the effects of different interfacial water structures. Wang et al. suggested the weakly hydrogen-bonded water formed an ordered structure with cations under biased potential, which facilitated the electron transfer and resulted in higher HER rates . Huang et al. argued that such a weakly hydrogen-bonded interfacial solvation environment increased the energy barrier of proton-coupled electron transfer and slowed down the kinetics of HOR/HER . Jia et al. proposed that the strongly hydrogen-bonded water with an oxygen-down (O↓) conformation accelerated rate of HOR/HER by shuffling reaction intermediates through Grotthuss mechanism . Despite the debate, tuning the interfacial water structures appears to be a promising new strategy to improve HOR catalysts. However, the interfacial water-catalyst interaction is largely non-covalent so it cannot be regulated by the electronic structures of catalysts . Methods to manipulate such interactions has rarely been proposed .