Thermotropic liquid crystals (LCs) present opportunities for synergistic interactions with ligand-functionalized nanoparticles (NPs). Understanding the dynamics and structures of ligand-coated NPs in an anisotropic LC environment allows for better design and control of versatile LC-NP hybrid materials. Here, simulations and experiments yield direct evidence that cyanobiphenyl LCs induce anisotropy in the biphenylalkyl ligand shells of spherical NPs. The ellipsoidal NP aligns with the LC director. Magnetic fields can dictate the directional ordering of mesogens and consequently allow control of the orientation of the nonmagnetic NPs. Controlling the alignment and deformation advances the design and engineering of these hybrid nanomaterials.

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