Mössbauer spectroscopy is a powerful tool for quantitative mineralogical analysis of Fe-bearing materials. The miniature Mössbauer spectrometer MIMOS II is a component of the Athena science payload launched to Mars in 2003 on both Mars Exploration Rover missions. The instrument has two major components: (1) a rover-based electronics board that contains power supplies, a dedicated central processing unit, memory, and associated support electronics and (2) a sensor head that is mounted at the end of the instrument deployment device (IDD) for placement of the instrument in physical contact with soil and rock. The velocity transducer operates at a nominal frequency of ∼25 Hz and is equipped with two 57Co/Rh Mössbauer sources. The reference source (∼5 mCi landed intensity), reference target (α-Fe2O3 plus α-Fe0), and PIN-diode detector are configured in transmission geometry and are internal to the instrument and used for its calibration. The analysis Mössbauer source (∼150 mCi landed intensity) irradiates Martian surface materials with a beam diameter of ∼1.4 cm. The backscatter radiation is measured by four PIN-diode detectors. Physical contact with surface materials is sensed with a switch-activated contact plate. The contact plate and reference target are instrumented with temperature sensors. Assuming ∼18% Fe for Martian surface materials, experiment time is 6–12 hours during the night for quality spectra (i.e., good counting statistics); 1–2 hours is sufficient to identify and quantify the most abundant Fe-bearing phases. Data stored internal to the instrument for selectable return to Earth include Mössbauer and pulse-height analysis spectra (512 and 256 channels, respectively) for each of the five detectors in up to 13 temperature intervals (65 Mössbauer spectra), engineering data for the velocity transducer, and temperature measurements. The total data volume is ∼150 kB. The mass and power consumption are ∼500 g (∼400 g for the sensor head) and ∼2 W, respectively. The scientific measurement objectives of the Mössbauer investigation are to obtain for rock, soil, and dust (1) the mineralogical identification of iron-bearing phases (e.g., oxides, silicates, sulfides, sulfates, and carbonates), (2) the quantitative measurement of the distribution of iron among these iron-bearing phases (e.g., the relative proportions of iron in olivine, pyroxenes, ilmenite, and magnetite in a basalt), (3) the quantitative measurement of the distribution of iron among its oxidation states (e.g., Fe2+, Fe3+, and Fe6+), and (4) the characterization of the size distribution of magnetic particles. Special geologic targets of the Mössbauer investigation are dust collected by the Athena magnets and interior rock and soil surfaces exposed by the Athena Rock Abrasion Tool and by trenching with rover wheels.