The Panoramic Camera (Pancam) on the Mars Exploration Rover Opportunity acquired visible/near‐infrared multispectral observations of soils and rocks under varying viewing and illumination geometries that were modeled using radiative transfer theory to improve interpretations of the microphysical and surface scattering nature of materials in Meridiani Planum. Nearly 25,000 individual measurements were collected of rock and soil units identified by their color and morphologic properties over a wide range of phase angles (0–150°) at Eagle crater, in the surrounding plains, in Endurance crater, and in the plains between Endurance and Erebus craters through Sol 492. Corrections for diffuse skylight incorporated sky models based on observations of atmospheric opacity throughout the mission. Disparity maps created from Pancam stereo images allowed inclusion of local facet orientation estimates. Outcrop rocks overall exhibited the highest single scattering albedos (≤0.9 at 753 nm), and most spherule‐rich soils exhibited the lowest (≤0.6 at 753 nm). Macroscopic roughness among outcrop rocks varied but was typically larger than spherule‐rich soils. Data sets with sufficient phase angle coverage (resulting in well‐constrained Hapke parameters) suggested that models using single‐term and two‐term Henyey‐Greenstein phase functions exhibit a dominantly broad backscattering trend for most undisturbed spherule‐rich soils. Rover tracks and other compressed soils exhibited forward scattering, while outcrop rocks were intermediate in their scattering behaviors. Some phase functions exhibited wavelength‐dependent trends that may result from variations in thin deposits of airfall dust that occurred during the mission.