This article reports the surface modification of electrospun polycarbonate urethane membrane with polydimethyl siloxane (PDMS) using plasma-induced grafting technique for biomedical applications. The nonwoven membranes were characterized for their structure, performance, and compatibility with cells. The surface modification was confirmed by means of attenuated total reflection Fourier transform infrared spectroscopy (ATR-FTIR) and energy dispersive X-ray analysis (EDXA). ATR-FTIR and EDXA analyses displayed characteristic absorption peaks of PDMS for the membrane. The structure and morphology of the developed membranes were studied using scanning electron microscope and microcomputed tomography (μCT). Scanning electron microscopy and μCT revealed the fibrous morphology and percentage porosity of the membranes before and after plasma modification. Static mechanical tests showed that the tensile strength was greater than 8 MPa. Physical characterization of the membranes after immersion in hydrolytic and oxidative media supports their biostability. Cytotoxicity of the membrane was evaluated using L929 fibroblast cells, and the results indicated that the membrane is cytocompatible. Accordingly, these results highlight the potential of this fibrous membrane for biomedical applications. © 2013 Wiley Periodicals, Inc.