1-Naphthyl-, 9-phenanthryl-, and 9-anthryl-substituted trialkyldisilenes 1-3 were synthesized as the first stable disilenes with single polycyclic aromatic substituents, allowing elucidation of the unprecedented intramolecular charge transfer interaction between disilene pi and aromatic pi systems. Anthryl-substituted disilene 3 having a low-lying pi*(aryl) LUMO showed a distinct ICT absorption band due to the charge transfer from a disilene pi donor to an aromatic pi acceptor.