Aligned carbon nanotube bundles (ACNTB) with multi-level hierarchical structures were tailored by reactive polymer vinyl-terminated polyphenylene ether (PPE) for the excellent integrated property of bismaleimide-triazine (BT) resin. The PPE-tailored ACNTB (ACNTB@PPE) has increased strength for the penetration of PPE into porous ACNTB strengthening the interaction between each CNT. The strong interaction at the interface of ACNTB@PPE and BT matrix can be created owing to the reaction of the vinyl group in PPE on the surface of ACNTB and maleimide group in BT. BT with 2% ACNTB@PPE composite shows the optimal flexural strength, fracture toughness and tensile strength, which are 88%, 115% and 77% higher than those of BT, respectively. The introduction of ACNTB@PPE slightly enhances the thermal property of BT. ACNTB@PPE can significantly improve the flame retardancy of BT composites. As compared to individual ACNTB, ACNTB@PPE effectively improves the integrated property of BT composites mainly due to the chemical interaction at the interface of ACNTB@PPE and BT matrix and the increased interaction between each CNT. (C) 2018 Elsevier B.V. All rights reserved.