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In this study, we investigated the impact of various simulated skull bone geometries on the determination of skull speed of sound and acoustic attenuation values via optimization using transmitted pressure amplitudes beyond the bone. Using the hybrid angular spectrum method (HAS), we simulated ultrasound transmission through four model sets of different geometries involving sandwiched layers of diploë and cortical bone in addition to three models generated from CT images of ex‐vivo human skull‐bones. We characterized cost‐function solution spaces for each model and, using optimization, found that when a model possessed appreciable variations in resolvable layer thickness, the predefined attenuation coefficients could be found with low error (RMSE < 0.01 Np/cm). However, we identified a spatial frequency cutoff in the models' geometry beyond which the accuracy of the property determination begins to fail, depending on the frequency of the ultrasound source. There was a large increase in error of the attenuation coefficients determined by the optimization when the variations in layer thickness were above the identified spatial frequency cutoffs, or when the lateral variations across the model were relatively low in amplitude. For our limited sample of three CT‐image derived bone models, the attenuation coefficients were determined successfully. The speed of sound values were determined with low error for all models (including the CT‐image derived models) that were tested (RMSE < 0.4 m/s). These results illustrate that it is possible to determine the acoustic properties of two‐component models when the internal bone structure is taken into account and the structure satisfies the spatial frequency constraints discussed. [ABSTRACT FROM AUTHOR]