Three new ternary selenidocadmates, K6[CdSe4] (1), K2[CdSe2] (2), and K2[Cd3Se4] (3), were synthesized and isolated upon fusion of K2Se and CdSe in respective stoichiometric amounts, followed by aminothermal treatment with 1,2‐diaminoethane. The anionic substructures range from molecules (0D, 1) through strands (1D, 2) to layered motifs (2D, 3). Compound 1 is isostructural to the corresponding mercury compound, K6[HgSe4], whereas the structure of 3 was previously predicted according to powder diffraction data, and could now be confirmed. The 1D chains in the anion of 2 represent a novel anionic architecture for this class of compounds. Determination of optical absorption properties confirm the expected decrease of the onset‐of‐absorption energies with increasing dimensionality of the anionic structures along the series of compounds. The structures of 1–3 were determined by means of single‐crystal Xray diffraction, and the heavy‐atom composition of the compounds was confirmed by micro Xray fluorescence spectroscopy (μ‐XFS).