Luminescent solar concentrators (LSCs) suffer greatly from reabsorption, where emitted light is parasitically reabsorbed by a luminophore. Specifically designed luminophores with inherently large Stokes shifts have been successfully synthesized in the literature; however, they introduce a new issue of poor absorption due to excessive blue shifting of the luminophores' absorption. Hybrid luminophores consisting of quantum dots (QDs) coupled to organic dyes offer a solution to this problem, by improving light sensitization and increasing the Stokes shift via energy transfer. We present a Cd/Pb-free InP/ZnS QD donor coupled to a rhodamine 101 acceptor hybrid luminophore LSC (10 × 10 × 0.3 cm, gain factor 8.33). The external quantum efficiency of the device under 405 nm illumination was 2.7 ± 0.6%, giving a mean 50% increase in external quantum efficiency relative to an InP/ZnS QD device. This study represents the first inorganic to organic hybrid nanomaterial system with attached luminophores in the solid state. We also perform an in-depth investigation by optical characterization of the different operational metrics of our novel LSCs.