Liquid-crystalline materials are a promising class of stimuli-responsive materials that have been demonstrated to undergo surface-induced orientational ordering transitions that can be highly sensitive and specific to chemical species. However, past studies demonstrating surface-induced transitions in liquid crystals (LCs) have employed thin films of low-molecular-weight LCs that are difficult to stabilize (due to dewetting of the LC on a surface). Here, it is reported that it is possible to prepare liquid-crystalline gels using a mixture of polystyrene microspheres and nematic LCs that undergo changes in orientational order, and thus optical appearance, in response to exposure to specific chemical compounds. These colloid-in-liquid-crystal (CLC) gels are mechanically stable and can be molded on chemically functionalized surfaces into thin films containing micrometer-sized LC-rich domains that span the two interfaces of the gels. In contrast to other reports of LC gels, where the presence of a polymeric or self-assembled small-molecule gelator network within a nematic LC frustrates ordering transitions from propagating through the gels over distances, it is demonstrated that thin films of CLC gels, when supported on chemically functionalized surfaces, do undergo easily visualized ordering transitions upon exposure to organophosphonate compounds. Because these optically responsive CLC gels are mechanically robust and can be molded, this class of composite LC material may be broadly useful for the design of chemically responsive LC devices.