The spin decomposition of a spin-contaminated different-orbitals-for-different-spins (DODS) wave function is formulated in terms of the Krylov space of the operator. The number of determinants that contribute to the various projected spin eigenfunctions depends on the sparsity of the orbital overlap matrix X between the α and β spatial orbitals. The cosine-sine decomposition (CSD) procedure may be applied to this overlap matrix, and the resulting redundant orbital transformations may be applied to the α and β spatial orbitals. This produces a sparse X′ matrix in the transformed basis in which each row or column has either one or two nonzero elements. This sparse X′ matrix simplifies the spin-decomposition procedure in three ways: 1) it reduces the number of contributing determinants within the Krylov basis functions and within the projected spin functions, 2) it reduces the effective orbital dimension through elimination of the frozen core and frozen virtual orbitals, and 3) it simplifies the spin-decomposition procedure in both the original and transformed bases by limiting the Krylov space dimension. These simplifications all reduce the computational effort for the spin-decomposition process. This procedure is implemented within a string-based DODS determinant formulation and applied to spin projection of unrestricted Hartree–Fock determinants.