Combining green preparation and high performance is becoming the direction of sustainable development of materials. How to simultaneously overcome the two bottlenecks (poor surface activity and UV resistance) of aramid fibers (AFs) while improving thermal and mechanical properties through a green process is still an interesting issue with big challenge. Herein, new AFs (BL-AFs) were prepared by alternately self-assembling SiO2 and MgAlFe layered double hydroxide (LDH) on surfaces of AFs, successively, through a green layer-by-layer (LBL) self-assembly technique without using high temperature and organic solvent. The structures and properties of BL-AFs were systematically studied, which are controllable by adjusting the number of self-assembly cycle. The new fibers with three or more self -assembly cycles have remarkably improved surface activity, thermal resistance, mechanical properties and UV resistance compared with AFs. Typically, with three self-assembly cycles, the initial degradation temperature and char yield of the new fiber (3BL-AF) are as high as 552.9 degrees C and 81.2%, about 92 degrees C and 25.2% higher than those of AF, respectively; after 168 h-UV irradiation, the retention of tensile performances of 3BL-AF fiber is as high as 91-95%, about 29-14% higher than that of AF, showing the best overall performances among all modified AFs prepared using a green technique reported so far. The origin behind the attractive performances of BL-AFs is revealed through correlating with structures of original and modified fibers. The excellent comprehensive properties of BL-AFs demonstrate that the green method provided in this study is facile and effective to completely solve the bottlenecks of aramid fibers, and developing higher performance organic fibers. (C) 2017 Elsevier B.V. All rights reserved.