This paper summarizes recent progress toward an emerging, unconventional application of thermotropic liquid crystals (LCs) - their use as solvents for controlling the assembly of non-LC nanoscale building blocks. LCs offer a number of potential advantages compared to conventional isotropic solvents, including the ability to influence building block orientation and other structural properties. Strategies are reviewed for the exploitation of LC media to engineer order in a range of systems, including oriented organic monolayers, chiral films, and nanometer-scale particles.