One of the most detrimental loss mechanisms in Luminescent Solar Concentrators (LSCs) is reabsorption of emitted light from the luminophore. Silicon Nanocrystals (SiNCs) offer a solution due to the high apparent Stokes shift, but the poor absorption properties limit their performance as LSC luminophores. Coupling an organic dye to SiNCs represents a smart approach to obtain sensitization of SiNC luminescence by the organic dyes, thus, resulting in tunable and improved optical properties of LSCs. In particular, 9,10-diphenylanthracene was employed as a UV sensitizer for SiNCs in order to produce LSCs with an aesthetic appearance suitable to smart window application and optical efficiency as high as 4.25%. In addition, the role of the energy transfer process on LSC performance was elucidated by a thorough optical and photovoltaic characterization.