The structure and rheological properties of xanthan gum (XG) modified in a cold plasma environment were investigated. XG was functionalized in a capacitively coupled 13.56-MHz radio frequency dichlorosilane (DS)-plasma conditions and, consecutively, in situ aminated by ethylenediamine. The surface structure of modified XG was evaluated on the basis of survey and high-resolution ESCA, FTIR, and fluorescence labeling techniques. The types of species generated in DS-plasma were reported using residual gas analysis (RGA). The aqueous solutions of modified XG were cross-linked and cured at room temperature to form stable gels. The dynamic rheological characteristics of virgin XG and functionalized and cross-linked XG were compared. It was found that parameters such as plasma treatment time and concentration of solutions can be optimized to form stable gels of XG. Thus, cold plasma technology is a novel, efficient, and nonenzymatic route to modify XG.