Introducing photochromic or polymeric dopants into nematic liquid crystals is a well-established method to create stimuli-responsive photonic materials with the ability to “control light with light”. Herein, we demonstrate a new material design concept by showing that specific supramolecular interactions between the host liquid crystal and the guest dopants enhance the optical performance of the doped liquid crystals. By varying the type and strength of the dopant–host interaction, the phase-transition temperature, the order parameter of the guest molecules, and the diffraction signal in response to interference irradiation, can be accurately engineered. Our concept points out the potential of supramolecular interactions in liquid-crystal photonics, being valuable for optimizing the design of dye-doped functional liquid-crystalline systems.