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Osmium complexes with osmium in different oxidation states (II, III, IV, and VI) have been reported to exhibit antiproliferative activity in cancer cell lines. Herein, we demonstrate unexplored opportunities offered by 187Os nuclear forward scattering (NFS) and nuclear inelastic scattering (NIS) of synchrotron radiation for characterization of hyperfine interactions and lattice dynamics in a benchmark Os(VI) complex, K2[OsO2(OH)4]. We determined the isomer shift [δ = 3.3(1) millimeters per second] relative to [OsIVCl6]2- and quadrupole splitting [ΔEQ = 12.0(2) millimeters per second] with NFS. We estimated the Lamb-Mössbauer factor [0.80(4)], extracted the density of phonon states, and carried out a thermodynamics characterization using the NIS data combined with first-principles calculations. Overall, we provide evidence that 187Os nuclear resonance scattering is a reliable technique for the investigation of hyperfine interactions and Os-specific vibrations in osmium(VI) species and is thus applicable for such measurements in osmium complexes of other oxidation states, including those with anticancer activity such as Os(III) and Os(IV). [ABSTRACT FROM AUTHOR]