Dielectric barrier discharge (DBD) plasma for the synthesis of Zr-MOFs followed by the calcination and combination with Cr-MOFs was presented to prepare a Brønsted-Lewis bifunctional catalyst for the conversion of glucose to 5-hydroxymethylfurfural (HMF). The strong electric field on the catalyst surface formed by DBD plasma induced the enhancement of strong metal oxide support interaction (SMOSI), which could be indicated by XPS. SMOSI could change the embedding degree of metal micro-particles. SMOSI accompanied with the encapsulation of Zr metal nanoparticles could regulate the acid sites of the catalysts. Lewis acid played an important role in the isomerization of glucose to fructose, while Brønsted acid played a key role in the further conversion of glucose. The strong Brønsted acid sites determined the conversion of glucose to HMF. Cr-MOFs@ZrO2-D with the DBD plasma method afforded a higher Brønsted to Lewis acid ratio, compared with Cr-MOFs@ZrO2-S with the hydrothermal method. Glucose conversion of 97.9 % and HMF yield of 38 % were obtained with DMF solvent system and Cr-MOFs@ZrO2-D at 150 °C for 2h. This research provided a new method for preparing Zr-MOFs by DBD plasma and a new idea to comprehensively understand the role of Brønsted and Lewis acid sites in glucose conversion.