| Summary: | The synthesis, structural, and photophysical investigations of CuI complexes with a disilanylene-bridged bispyridine ligand <b>1</b> are herein presented. Dinuclear (<b>2</b>) and ladder-like (<b>3</b>) octanuclear copper(I) complexes were straightforwardly prepared by exactly controlling the ratio of CuI/ligand <b>1</b>. Single-crystal X-ray analysis confirmed that dinuclear complex <b>2</b> had no apparent π…π stacking whereas octanuclear complex <b>3</b> had π…π stacking in the crystal packing. In the solid state, the complexes display yellow-green (<i>λ</i><sub>em</sub> = 519 nm, <i>Φ</i> = 0.60, <i>τ</i> = 11 µs, <b>2</b>) and blue (<i>λ</i><sub>em</sub> = 478 nm, <i>Φ</i> = 0.04, <i>τ</i> = 2.6 µs, <b>3</b>) phosphorescence, respectively. The density functional theory calculations validate the differences in their optical properties. The difference in the luminescence efficiency between <b>2</b> and <b>3</b> is attributed to the presence of π…π stacking and the different luminescence processes.
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