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We report the synthesis and characterization of a symmetric dinucler DyIIIcomplex (1) based on the use of bulk pentapyridyldiamine (BPA-TPA) and bridging hydroquinone ligands. Each DyIIIion is wrapped by a BPA-TPA ligand, leaving only one site to bond one O donor atom from the hydroquinone, which generates a triangular dodecahedral coordinate geometry. Magnetic measurements reveal that complex 1exhibits a high anistropy barrier of 727(4) K and the temperature of hysteresis loops up to 20 K with remanence at the zero field. However, the Y(III)-diluted analogue 1@Yshows that butterfly-shaped hysteresis loops are closed at the zero field. This discrepancy clearly demonstrates the positive effect of axial magnetic interaction between the DyIIIdimer. The fascinating behavior is ascribed to the pseudolinear ligand field with an exceptionally short Dy–O bond, as confirmed by theoretical calculations.