Polysaccharides are abundant components in Pu-erh tea, yet the utilization of insoluble polysaccharides under the actions of microbiota has rarely been studied. The aim of this work was to study how insoluble polysaccharides were utilized during fermentation through the investigation of the variations and correlation of microbiota with polysaccharides degradation products. Genomics study revealed the significant changes of microbiota. Metabolomics analysis showed monosaccharides (types 1 and 3) were consumed during early and middle fermentation stages, while carboxylic acids and other monosaccharides (type 2) were accumulated at middle and late pile-fermentation stages. Correlation revealed that type 1 and 3 monosaccharides, which act as energy providers, were positively associated with Aspergillus, while type 2 monosaccharides possessing multiple bioactivities and carboxylic acids influencing tea taste were positively related to Rasamsonia, Thermomyces, Bacillaceae, and Lactobacillaceae. This study would be beneficial to improve production efficiency and provide basis for quality control of Pu-erh tea fermentation.