We report high frequency electron paramagnetic resonance (EPR) investigations of a series of high spin (total spin up to S = 10) manganese and nickel complexes which have been shown to exhibit single molecule magnetism, including low temperature (below ∼ 1K) hysteresis loops and resonant magnetic quantum tunneling. A cavity perturbation technique enables high sensitivity oriented single crystal EPR measurements spanning a very wide frequency range (16 to 200+ GHz). Fitting of the frequency and field orientation dependence of EPR spectra allows direct determination of the effective spin Hamiltonian parameters. Studies on a range of materials with varying (approximately axial) site symmetries facilitates an assessment of the role of transverse anisotropy (terms in the Hamiltonian that do not commute with ŝz) in the magnetic quantum tunneling phenomenon.