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Determining the roles of surface functionality of heterogeneous acid catalysts is important for many industrial catalysts. In this study, the decisive structure of metal-organic frameworks (MOFs) is utilized to identify important features for the effective conversion of d-xylose into lactic acid. Several acidic MOFs are tested and the combination of Lewis acidity and adjacent hydroxy sites is found to be critical to attain high lactic acid yields. This hypothesis is corroborated experimentally by modification of the MOF to increase such sites, which affords an enhanced lactic acid yield of 79 %, and investigation of the acidity by using in situ FTIR spectroscopy. Density functional theory calculations disclose the cooperative behavior of Lewis acid sites and hydroxy groups in promoting the Cannizzaro reaction, a key step in the production of lactic acid., (© 2022 Wiley-VCH GmbH.)