The adsorption is widely used to remove dyes from wastewater because of its low cost, simple preparation, and environmental friendliness. However, the existing adsorbents suffer from difficult recycling, inconvenient use, and low regeneration rate. In this study, polyacrylonitrile (PAN) and graphene oxide (GO) was mixed for electrospinning GO/PAN nanofiber membrane and then chitosan (CS) was grafted to obtain CS-GO/PAN nanofiber membrane. CS-GO/PAN membrane were characterized with FE-SEM, EDX, FT-IR and, WCA. The effects of membrane types, dosage, solution pH on the removal of dye sunset yellow (SY) were systematically investigated. The results showed that more than 80% of SY were removed within 15 min at pH 2 using 100 mg CS-GO/PAN membrane. Adsorption kinetic data were fitted well with the pseudo-second-order model and adsorption equilibrium achieved within 240 min. The isotherm study followed the Langmuir model with the actual maximum adsorption capacity of 211.54 mg/g. After 5 adsorption-desorption cycles, the adsorption efficiency and the desorption efficiency of CS-GO/PAN were over 90% and 93%, respectively. Moreover, the membrane recovered easily from the water while its integrity was still maintained. The CS-GO/PAN membrane demonstrates the virtue of high adsorption capacity, easy operation, and good reusability, which could be considered as a promising material for adsorbing dyes in wastewater.