We show the pseudospectral method is a powerful tool for finding precise solutions of Schrödinger's equation for two-electron atoms with general angular momentum. Realizing the method's full promise for atomic calculations requires special handling of singularities due to twoparticle Coulomb interactions. We give a prescription for choosing coordinates and subdomains whose efficacy we illustrate by solving several challenging problems. One test centers around the determination of the nonrelativistic electric dipole oscillator strength for the helium 1 1 S → 2 1 P transition. The result achieved, 0.27616499 (27), is comparable to the best in the literature. The formally equivalent length, velocity, and acceleration expressions for the oscillator strength all yield roughly the same accuracy. We also calculate a diverse set of helium ground state expectation values, reaching near state-of-the-art accuracy without the necessity of implementing any specialpurpose numerics. These successes imply that general matrix elements are directly and reliably calculable with pseudospectral methods. A striking result is that all the relevant quantities tested in this paper -energy eigenvalues, S-state expectation values and a bound-bound dipole transition between the lowest energy S and P states -converge exponentially with increasing resolution and at roughly the same rate. Each individual calculation samples and weights the configuration space wave function uniquely but all behave in a qualitatively similar manner. These results suggest that the method has great promise for similarly accurate treatment of few-particle systems.