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The electronic structures within a series of square‐planar ruthenium(II) pincer complexes with dialkyl‐, vinyl alkyl‐, and divinyl amido pincer backbones is compared in an experimental and computational study. Although [RuCl{N(CH2CH2PtBu2)2}] exhibits a low‐spin (S=0) ground state and low‐lying triplet (S=1) excited state, [RuCl{N(CH2CH2PtBu2)(CHCHPtBu2)}] and [RuCl{N(CHCHPtBu2)2}] adopt intermediate‐spin (S=1) ground states with strong magnetic anisotropy due to large zero‐field splitting (D>+200cm–1). The change in ground‐state electronic configuration is attributed to tailored pincer ligand‐to‐metal π‐donation within the PNP ligand series. For more details, see the Full Paper by S. Schneider et al. on page 579 ff. [ABSTRACT FROM AUTHOR]