A new method is introduced for the optimization of nonorthogonal virtual orbitals for use in general multiconfiguration spin-coupled wave functions. The use of a number of highly effective approximations greatly reduces the computational effort involved, the most important being the use of a second-order perturbation expression for the energy and an approximate expression for the elements of the Hessian. As a result, the overall scheme scales very favourably with respect to the numbers of active electrons and of basis functions, making it suitable for the accurate study of large systems. Benchmark calculations are presented for the dissociation of LiH(X1Σ+) and Li2(X1Σ+ g ) using a highly compact four-configuration wave function. Standard spin-coupled valence bond expansions in the same virtual space are required to be significantly larger before equivalent results are obtained. The results are shown to compare very favourably with full valence complete active space self-consistent field calculations using an identical basis, and binding energies are within 4% of the values obtained from full configuration interaction calculations in the same basis set.