Integrated paramagnetic resonance, utilizing electron paramagnetic resonance (EPR), NMR, and electron-nuclear double resonance (ENDOR), of a series of cobalt bis-trispyrazolylborates, Co(TPx)(2), are reported. Systematic substitutions at the ring carbons and on the apical boron provide a unique opportunity to separate through-bond and through-space contributions to the NMR hyperfine shifts for the parent, unsubstituted Tp complex. A simple relationship between the chemical shift difference (delta(H) - delta(Me)) and the contact shift of the proton in that position is developed, This approach allows independent extraction of the isotropic hyperfine coupling, A(iso) for each proton in the molecule. The Co center dot center dot H contact coupling energies derived from the NMR, together with the known metrics of the compounds, were used to predict the ENDOR couplings at g(perpendicular to). Proton ENDOR data is presented that shows good agreement with the NMR-derived model. ENDOR signals from all other magnetic nuclei in the complex (N-14, coordinating and noncoordinating, B-11 and C-13) are also reported.