P-31 and Co-59 NMR have been applied to study the structure and dynamics of the tetrahedral mixed-metal cluster HFeCO3(CO)(9)[P(OCH3)(3)](3) both in the solid state and in solution. The P-31 chemical shift (CS) anisotropy, the direct (D) and indirect (J) dipolar P-31-Co-59 interactions, and the relative orientation of the CS, D, and J tensors have been determined by iterative fitting of the P-31 MAS NMR spectra at two magnetic field strengths (4.7 and 7.1 T). The quadrupole coupling constant as well as the isotropic part and anisotropy of the CS tensor at the Co-59 nucleus has been evaluated by a moment analysis of the solid-state central transition line shape. The P-31 and Co-59 NMR data, which are both influenced by second-order quadrupolar shifts, clearly show a departure from the C-3 upsilon molecular symmetry due to a solid-state packing effect. Using the static interaction parameters obtained by solid-state NMR, it was possible to evaluate the overall rate of molecular motion in solution from Co-59 relaxation measurements. The analysis of the solution-state P-31 NMR saddle-shaped spectrum gives the same (1)J(P-31-Co-59) coupling constant as in the solid state. Moreover, no Q-CS relaxation interference effects are detected in agreement with the very weak contribution of the CS anisotropy to the Co-59 relaxation predicted by the solid-state NMR data.