In this paper, poly(diallyl dimethyl ammonium chloride) (PDADMAC)-grated cellulose filter membranes (cellulose-g-PDADMAC) were fabricated via atom transfer radical polymerization (ATRP) for selective removal of anionic dye from wastewater. Gel permeation chromatography (GPC), X-ray photoelectron spectroscopy (XPS), and Fourier transform infrared spectroscopy (FTIR) showed that PDADMAC was grafted onto the filter membrane surface via a controllable living polymerization. The resultant cellulose-g-PDADMAC membranes exhibit selective removal for anionic methyl orange (MO) through rapid and facile filtration using model MO/rhodamine B (RB) mixture, due to the electrostatic interaction between quaternary ammonium groups of membrane and the sulfonic groups of MO. The decolorization ratio of MO remains higher than 95% when the graft ratio is 13.3% even after 6 cycles. Cellulose-g-PDADMAC also shows effective antimicrobial activities against S. aureus and E. coli. The modified filter membranes are promising for the potential application in wastewater purification. PDADMAC-grated cellulose filter membranes with good recyclability and high antimicrobial activity were fabricated via atom transfer radical polymerization for selective removal of anionic dye from wastewater.