The simple shear response of soft polymers under large deformation (>50%) and strain rates spanning 10 −3 – 10 3 s −1 is characterized by developing quasi-static and split-Hopkinson pressure bar based single-pulse dynamic simple shear experiments rooted in continuum mechanics fundamentals. Cross-linked polydimethylsiloxane (PDMS) is chosen as a model material. By examining the evolution of stress, strain and strain rate, the latter two parameters measured using two-dimensional digital image correlation (DIC), it is demonstrated that dynamic simple shear deformation consists of four distinct stages: momentum diffusion, inertia effect, steady-state material response, and strain rate decay. By isolating the unsteady and steady-state deformation stages, inertia-free material response is captured under a uniform strain rate. It is shown that the shear response of PDMS is nearly linear with a weakly rate-sensitive shear modulus in the investigated strain rate range. Further, by analyzing the DIC strain-field and comparing the kinematic experimental results with those predicted by classical continuum mechanics, it is demonstrated that the proposed experiments not only achieve a nearly theoretical simple shear state that is uniform across the specimen, but also allow for post-test validation of individual experiments based on these criteria. © 2019, Society for Experimental Mechanics.