An investigation of the mechanical strain rate, inelastic behavior, and microstructural evolution under deformation for an as-cast pearlitic gray cast iron (GCI) is presented. A complex network of graphite, pearlite, steadite, and particle inclusions was stereologically quantified using standard techniques to identify the potential constituents that define the structure–property relationships, with the primary focus being strain rate sensitivity (SRS) of the stress–strain behavior. Volume fractions for pearlite, graphite, steadite, and particles were determined as 74%, 16%, 9%, and 1%, respectively. Secondary dendrite arm spacing (SDAS) was quantified as 22.50 μm ± 6.07 μm. Graphite flake lengths and widths were averaged as 199 μm ± 175 μm and 4.9 μm ± 2.3 μm, respectively. Particle inclusions comprised of manganese and sulfur with an average size of 13.5 μm ± 9.9 μm. The experimental data showed that as the strain rate increased from 10−3 to 103 s−1, the averaged strength increased 15–20%. As the stress state changed from torsion to tension to compression at a strain of 0.003 mm/mm, the stress asymmetry increased ∼470% and ∼670% for strain rates of 10−3 and 103 s−1, respectively. As the strain increased, the stress asymmetry differences increased further. Coalescence of cracks emanating from the graphite flake tips exacerbated the stress asymmetry differences. An internal state variable (ISV) plasticity-damage model that separately accounts for damage nucleation, growth, and coalescence was calibrated and used to give insight into the damage and work hardening relationship.