Nitrogen removal and microbial interactions in two combined nitritation and Anammox systems with or without the addition of organics were examined. Two systems were successfully started up by adopting intermittent aeration. Organics addition deteriorated nitrogen removal, and total inorganic nitrogen and ammonium removal percentages decreased by 16.4% and 26.3%, respectively. Organics addition promoted the growth of Chloroflexi and Proteobacteria while suppressed the growth of Candidatus Kuenenia. Organics addition decreased activities of fatty acid biosynthesis and metabolism, amino acid metabolism and biofilm formation, while increased activities of steroid metabolism and glycosaminoglycan biosynthesis. Heterotrophs and Candidatus Kuenenia might interact with other organisms by using diverse quorum sensing systems. Chloroflexi and Proteobacteria interacted with Candidatus Kuenenia in nitrogen metabolism and biofilm formation. Proteobacteria played a key role in building a nitrite loop with Candidatus Kuenenia and nitrifiers. These results clarified microbial interactions in the autotrophic nitrogen removal process and advance its application.