This study investigated the effects of LAB inoculants (L) and molasses (M) on the microbial community and fermentation quality of cassava foliage (CF). The small segments (about 2-3 cm) CF were ensiled in plastic bags and incubated at normal temperature (25°C). Four treatments were carried out as follows: control (no additives, CK), LAB inoculants (Lactobacillus plantarum, L), molasses (M), and LAB in combination with molasses (LM). The LAB and molasses obviously altered the bacterial community structure of the CF silage and enhanced the fermentation quality. The combination addition could increase the abundance of Lactobacillus and reduce the Pseudomonas. The LAB and molasses also significantly elevated the lactic acid concentration (P < 0.001) and decreased the pH (P < 0.001), as well as the concentrations of acetic acid, propionic acid, butyric acid, and ammonia-N (P < 0.05). In addition, the combination treatment displayed more effective results on silage fermentation. The LAB and molasses improved the fermentation quality of the CF silage by altering the bacterial community structure. Furthermore, the bacterial community was significantly correlated with fermentation indexes.