The Lagrange-based Grassmann interpolation (G-Int) method has been extended for open-shell systems using restricted open-shell (RO) methods. The performance of this method was assessed in constructing potential energy surfaces (PESs) for vanadium(II) oxide, benzyl radical, and methanesulfenyl chloride radical cation. The density matrices generated by G-Int when used as initial guesses for self-consistent field (SCF) calculations, exhibit superior performance compared to other traditional SCF initial guess schemes, such as SADMO, GWH, and CORE. Additionally, the energy obtained from the G-Int scheme satisfies the variational principle and outperforms the direct energy-based Lagrange interpolation approach. In the case of methanesulfenyl chloride radical cation, a unique example with a flat PES at the end region along the H-C-S-Cl dihedral angle, the use of an equally-spaced grid sampling leads to significant oscillations near the end of the interval due to the effects of Runge's phenomenon. Introducing an unequally-spaced grid sampling based on a scaled Gauss-Chebyshev quadrature effectively mitigated the Runge's phenomenon, making it suitable for combining with G-Int in constructing PESs for general applications. Thus, G-Int provides an efficient and robust strategy for building spin contamination-free PESs with consistent accuracy.