Assembly techniques for graphene have attracted intense attention since their performance strongly depends on the manners in which graphene nanosheets are arranged. In this work, we demonstrate a viable process to synthesize winged graphene nanofibers (G-NFs) which can effectively prevent the inter-sheet restacking and thus enhance their performance in electrochemical energy storage by the wings on the fibers. The G-NF frameworks were achieved by processing the precursor graphene oxide nanosheets with the following procedures: microwave irradiation, salt addition, freeze-drying, and chemical reduction. The resultant frameworks are composed of winged G-NFs with a diameter of 200-500 nm and a length of 5-20 µm. Moreover, the crimp degree of G-NFs can be rationally controlled by microwave irradiation time. A formation mechanism of such winged G-NFs based on the synergistic effects from MW irradiation and solution ionic strength change has been proposed. With a practice in flexible electrode, after decorated with amorphous MnO2, the G-NF frameworks shows an enhanced specific capacitance compared to graphene nanosheets (G-NSs). This research has developed a controllable method for G-NF assembly to avoid the restacking of G-NSs, which might highly enhance their performance in supercapacitor and related fields.