The cross-polarization isolation (CPI) is a key parameter to assess the dual-polarization antenna because the cross-polarization closely affects the antenna application. A polarization state configuration (PSC) approach is proposed to configure the polarization state of the polarimetric phased array radar antenna. Unlike the traditional fixed polarization states such as the linear polarization (LP) and the circular polarization (CP), the PSC method modulates the polarization state of the radiated wave continuously. In addition, the optimal excitation magnitude and phase of the dual-polarization element is calculated, thereby maximizing the CPI. Most of the configured polarization state is the elliptical polarization (EP), and a lower cross-polarization level and higher CPI could be obtained. This method could expand the acceptable angle range when compared with the LP and CP waves. Numerical simulations and comparisons are conducted to manifest the validity of the proposed method.