Anaerobic digestion is an important technology to receive energy from various types of biomass. In this work, the impact of granular activated carbon (GAC) on the mesophilic anaerobic co-digestion of sugar beet pulp and distillers grains was investigated. After a short period, anaerobic reactors began to produce biomethane and were ready for completion within 19−24 days. The addition of GAC to reactors (5−10 g L−1) significantly enhanced the methane production rate and consumption of produced volatile fatty acids. Thus, the maximum methane production rate increased by 13.7% in the presence of GAC (5 g L−1). Bacterial and archaeal community structure and dynamics were investigated, based on 16S rRNA genes analysis. The abundant classes of bacteria in GAC-free and GAC-containing reactors were Clostridia, Bacteroidia, Actinobacteria, and Synergistia. Methanogenic communities were mainly represented by the genera Methanosarcina, Methanoculleus, Methanothrix, and Methanomassiliicoccus in GAC-free and GAC-containing reactors. Our results indicate that the addition of granular activated carbon at appropriate dosages has a positive effect on anaerobic co-digestion of by-products of the processing of sugar beet and ethanol distillation process.