This study investigated the performance of anaerobic digestion systems using four types of fibrous biofilm carriers, a polypropylene, a polyester, a polyamide, and a polyurethane fiber material. The biogas and methane production, pH, chemical oxygen demand, total solids content, volatile solids content, residual coenzyme F420, and microbial community compositions were determined during the experimental runs. Furthermore, scanning electron microscopy was employed to identify the microbial consortium and examine their attachment onto the surface of the four fibrous biofilm carriers. The polypropylene fiber system maintained the highest biogas and methane production in the reactor, which was 44.80% and 49.84% higher than that noted in the control, respectively, during the entire anaerobic fermentation cycle. Meanwhile, the polypropylene fiber system exhibited the highest TS, VS, and COD removal efficiency. The results of high-throughput sequencing indicated that the dominant species in the polypropylene fiber system were Methanoregula and Methanobacterium.