Understanding the bonding in transition metal complexes with redox-active ligands is a major challenge, for example in redox catalysis or in bioinorganic chemistry. In this work, electronic g-tensors, spin-density distributions, and electronic structure have been studied by different density functional methods for an extended series of complexes [Ru(acac)(2)(L)](n) (n = -1, 0, +1; L = redox-active o-quinonoid ligand). Comparison is made with experimental g-tensors and g-tensor-based oxidation-state assignments for a number of experimentally studied examples, using both gradient-corrected (BP86) and hybrid functionals (B3LYP, BHLYP) representing a range of exact-exchange admixtures. Reasonable, albeit not perfect, agreement with experimental g-tensors is obtained in one-component DFT calculations with hybrid functionals. Analyses of spin densities confirm the assignment of the cationic complexes as predominantly d(5)-Ru-III with a neutral quinonoid ligand. However, this conclusion is obtained only after inclusion of the appreciable spin polarization of the unrestricted determinant, while the singly occupied molecular orbital (SOMO) is localized more on the acac ligands. The anionic complexes turn out to be approximately halfway between a d(6)-Ru-II/semiquinone and a d(5)-Ru-III/catecholate formulation, but again only after taking into account the extensive spin polarization. Even the previous assignment of the neutral parent systems as d(5-)Ru(III)/semiquinone is not accurate, as a d(6)-Ru-II/quinone resonance structure contributes to some extent. Very unusual trends in the spin contamination of the Kohn-Sham determinant with increasing exact-exchange admixture in some of the cationic complexes have been traced to an interplay between spin delocalization and spin polarization.