Development of simultaneous nitrification-denitrification (SND) is a promising approach for nitrogen-rich water purification. Coupling biofilm reactors with novel biodegradable carrier of Pumelo Peel (PP) and various conventional plastic fillers (polyurethane filler, SPR-1 suspension filler, TA-II elastic filler and sphere filler) were examined to achieve SND in this study. Results represented that partially coupled with PP could achieve highly efficient SND. Optimal performance appealed in a bioreactor of coupling PP and SPR-1filler with ammonia and total nitrogen removal efficiencies of 96.8±4.0% and 78.9±9.5%, respectively, as well as low effluent CODMn of 1.85±0.86mgL-1. Notably, PP and conventional plastic filler played obviously different roles in combined bioreactor system. Microbial analysis suggested that dominant genera were Thiothrix, Gemmata, unclassified comanonadaceae, unclassified Rhizobiales, Salipiger, Chloronema and Klebsiella in optimal combined bioreactor, which indicated novel co-existence of heterotrophic nitrification, solid-phase, non-solid-phase heterotrophic and sulfur-based autotrophic denitrification for achieving efficient SND.