Responses of microbial communities to nanotoxicity in aquatic ecosystems are largely unknown, particularly with respect to relationship between community dynamics and functions. Here, periphytic biofilms were selected as a model of species-rich microbial communities to elucidate their responses when exposed to titanium dioxide nanoparticles (TiO2-NPs). Especially, the relationships between the functions (e.g. organic matter and Cu2+ removal) and community dynamics after long-term exposure to TiO2-NPs were assessed systematically. After 5days exposure to TiO2-NPs (5mgL-1), periphytic biofilms showed sustainable functions in pollutant removal and strong plasticity in defensing the toxic disturbance of TiO2-NPs, including photosynthesis and carbon metabolic diversity. The sustainable pollutant removal functions of periphytic biofilms were attributed to their functional redundancy. Specifically, periphytic biofilms altered their composition with cyanobacteria, Sphingobacteriia and Spirochaetes being the newly dominant taxa, and changed the carbon substrate utilization pattern to maintain high photosynthesis and metabolic rates. Moreover, extracellular polymeric substances (EPS) especially proteins were overproduced to bind the NPs and thereby reduce the nanotoxicity. The information obtained in this study may greatly help to understand the interactions between microbial community dynamics and function under NPs exposure conditions and functional redundancy is an important mechanism of periphytic biofilms to maintain sustainable functions.