The conventional characterization of work-hardening is to approximate the stress-strain diagram using the empirical curve-fitting of Hollomon or Voce. The new method uses the Taylor slip analyses to derive a functional form which is optimally fitted to the data. This constitutive relations analysis (CRA) duplicates the data using at least two fit loci. The fit parameters relate to the slip motion within the microstructure and hence its interpretation reveals the possible dynamic shape-change reactions. The fit-process defines a new yield stress which separates the yielding from the deformation mechanisms at large strains that breaks up into two regions separated by intersection parameters. The applications of CRA to nanovoid formation and growth leading to ductile failure, plane stress yield locus prediction using tensile tests and decoding the stress-strain diagram for age-hardened aluminum alloys have been successful. Using super-pure aluminum, this study confirms that CRA is based on crystal plasticity principles and that CRA can predict the correlation of the obstacle strength factor, α, with work-hardening, hence permitting conversion of flow stress at given strains to obstacle density. The derived results show that the inherent annihilation process and the changing strength factor are coordinated to result in a self-consistent constitutive relation.