Owing to the thermodynamics of surface melting described above, theoretical structure search workflows are expected to provide substantial insights into experimental synthesis in the future. Specifically, after predicting a superhydride structure, one can (i) calculate the pressure dependence of hydrogenation reaction enthalpy and (ii) estimate the melting point of the product to evaluate its feasibility for subsequent experiments. Although constructing MLPs for interfacial reactions, as in this study, is timeconsuming, workflows for bulk systems have already been established . Therefore, it is straightforward to develop MLPs for a homogeneous bulk system and estimate a rough melting temperature from the temperature-dependent enthalpy calculations. Consequently, we expect that the guiding principles derived from hydrogenation reactions via surface melting in our MLP-MD simulations, (i) the pressure dependence of hydrogenation reaction enthalpies and (ii) the melting temperature of superhydride products, significantly accelerate the synthesis of new superhydrides, integrating them with conventional computational techniques.