The coupling effect between nitrogen-vacancies (VN) and aluminum-interstitial sites (Ali) is investigated theoretically and experimentally in AlN helices. First-principles calculations predict a photoluminescence emission peak at approximately 600 nm in AlN doped with complex-defect (VNAli). A typical long afterglow (persistent luminescence) was observed in unintentionally doped AlN helices by introducing the complex-defect of (VNAli). An analysis of the luminescent characteristics indicated that the mechanism behind this afterglow is the complex-defect level and complex-defect density. These findings may further enrich the thoughts of defects in the wide band gap semiconductor of AlN.