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The single‐molecule magnet (SMM) properties of the isocarbonyl‐ligated dysprosium metallocene [Cp*₂Dy{μ‐(OC)₂FeCp}]₂ (1_Dy), which contains a rhombus‐shaped Dy₂Fe₂ core, are described. Combining a strong axial [Cp*]⁻ ligand field with a weak equatorial field consisting of the isocarbonyl ligands leads to an anisotropy barrier of 662 cm⁻¹ in zero applied field. The dominant thermal relaxation pathways in 1_Dy involves at least the fourth‐excited Kramers doublet, thus demonstrating that prominent SMM behavior can be observed for dysprosium in low‐symmetry environments.