We present an optimized luminescent solar concentrator (LSC) based on the combination of different organic dyes as luminescent species and silicon solar cells. As a first part of this work, a deep screening of organic dyes used since the 1980s in LSC research has been performed and 14 of them have been chosen and characterized in a polymethyl methacrylate (PMMA) host at a fixed concentration (1%). Departing from this initial study, an empirical optimization procedure has been implemented, aiming the highest photon collection at the edges of the LSC plate under a solar AM1.5G spectrum. An optimal three-dye system has been selected in order to achieve a high absorption range over the uv–vis spectrum. The incorporation of these molecules in the PMMA host has been made following two different strategies: (i) the stacking of three individual LSC plates (one dye in each) and (ii) the merging of three organic dyes in a single LSC plate allowing Förster resonance energy transfer (FRET) to occur. In addition, PMMA bulk and thin film on glass plates have been manufactured considering stacking and FRET strategies. Finally, a bulk FRET-based LSC has been manufactured and its optical and electrical performance evaluated and compared to the best reported values used for LSC characterization. To the best of our knowledge, our LSC possesses the highest reported concentration (), surpassing Slooff et al. ().