A suite of experimentally deformed single-crystal pyrite samples has been investigated using electron backscatter diffraction (EBSD). Single crystals were loaded parallel to <100> or <110> and deformed at a strain rate of 10-5 s-1, confining pressure of 300 MPa and temperatures of 600°C and 700°C. Although geometrically (Schmid factor) the {001}<100> slip system should not be activated in <100> loaded samples, lattice rotation and boundary trace analyses of the distorted crystals indicate this slip system is easier to justify. Determination of 75 MPa as the critical resolved shear stress (CRSS) for {001}<100> activation, in the <110> loaded crystals, suggests a crystal misalignment of ~5—15° in the <100> loaded crystals would be sufficient to activate the {001}<100> slip system. Therefore, {001}<100> is considered the dominant slip system in all of the single-crystal pyrite samples studied. Slip-system analysis of the experimentally deformed polycrystalline pyrite aggregates is consistent with the single-crystal findings, with the exception that {001}<11̄> also appears to be important, although less common than the {001}<100> slip system. The lack of crystal preferred orientation (CPO) development in the polycrystalline pyrite aggregates can be accounted for by the presence of two independent symmetrically equivalent slip systems more than satisfying the von Mises criterion.