A luminescent solar concentrator (LSC) is a potential low-cost enhancement of the standard large-area silicon photovoltaic panels for the generation of electricity from sunlight. In this work, guest-host systems are investigated using anisotropic fluorescent dyes and liquid crystal mesogens to control the direction of emitted light in the LSC. It is determined that up to 30% more light is emitted from the edge of an LSC waveguide with planar dye alignment parallel to the alignment direction than from any edge of an LSC with no alignment (isotropic). The aligned samples continue to show dichroic performance after additions of both edge mirrors and rear scattering layer.