Obtaining precise parameters of deformation modes remains a significant challenge in materials science research. Critical resolved shear stresses (CRSS) and work hardening, particularly in hexagonal metals, are crucial parameters for constitutive laws in crystal plasticity. This paper presents a novel approach to determine CRSS and specific hardening matrix coefficients for commercially pure zirconium (α-Zr) at room temperature. In situ methods are employed to measure displacement fields using grids applied to the sample surface, while a comprehensive characterization of the activated deformation systems is performed via SEM and TEM. The CRSS for prismatic ⟨a⟩, pyramidal ⟨a⟩, and {10 12} and {11 21} twinning systems, as well as the self-hardening for prismatic slip and several work-hardening coefficients (for prismatic/prismatic and prismatic/pyramidal interactions), are reported in Zr single crystals. Finally, the results are compared with findings from the literature and atomistic simulations.