The dehydration of carbohydrates to 5-hydroxymethylfurfural (HMF) is still a major challenge in the bioenergy industry. In this study, metal-containing silicoaluminophosphate molecular sieves (MeSAPO-5) with different Si/Al ratios were first synthesized from attapulgite by the hydrothermal method and applied to the dehydration of carbohydrate. The morphology, structure, and acid properties of MeSAPO-5 molecular sieves were studied by XRD, SEM, EDX, TG/DTA, pyrolysis IR (Py-IR), and NH3-TPD. The results indicated that MeSAPO-5 catalyst with Si/Al ratio of 0.25 provided much more acid active sites for feasible accessibility of HMF, after partial Al atoms were substituted by Si and Me atoms. The further increase of Si/Al ratio resulted in the decrease of the acidity of the molecular sieves, which significantly influenced their catalytic performance. Over the MeSAPO-5(0.25Si) catalyst, the HMF yield of 73.9% was obtained at 170 degrees C with 2.0 h. This indicated that MeSAPO-5 molecular sieves were a fairly promising catalyst for the carbohydrates dehydration to HMF.