Microbial enzymes are crucial for material biotransformation during the composting process. In this study, we investigated the effects of adding bamboo charcoal (BC) (i.e., at 5%, 10%, and 20% corresponding to BC5, BC10, and BC20, respectively) on the enzyme activity levels during chicken manure composting. The results showed that BC10 could increase the cellulose and urease activities by 56% and 96%, respectively. The bacterial community structure in BC10 differed from those in the other treatments, and Luteivirga, Lactobacillus, Paenalcaligenes, Ulvibacter, Bacillus, Facklamia, Pelagibacterium, Sporosarcina, Cellvibrio, and Corynebacterium had the most important roles in composting. Compared with other treatments, BC10 significantly enhanced the average rates of degradation of carbohydrates (D-xylose (40%) and α-D-lactose (44%)) and amino acids (L-arginine (16%), L-asparagine (14%), and L-threonine (52%)). We also explored the associations among the bacterial community and their metabolic functions with the changes in the activities of enzymes. Network analysis demonstrated that BC10 altered the co-occurrence patterns of the bacterial communities, where Ulvibacter and class Bacilli were the keystone bacterial taxa with high capacities for degrading carbon source, and they were related to increases in the activities of cellulase and urease, respectively. The results obtained in this study may help to further enhance the efficiency of composting.