A new azobenzene‐group‐containing monomer and several respective functional side‐chain polymers grafted on a methylhydrosiloxane backbone (with two different degrees of poly­merization; with and without the addition of a photoreactive benzophenone derivative) are designed, synthesized, and characterized. The resulting materials clearly show self‐assembly behavior and possess a nematic liquid‐crystal phase over a broad temperature range, which extends below 0 °C. The optical properties of these new photo­chromic liquid‐crystalline materials are determined from the absorbance spectra of oriented samples and by photo­induced birefringence studies. The results indicate a considerable dichroism of the side‐chain liquid‐crystalline polymers (SCLCPs), and hence demonstrate their potential applicability for optical storage.

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