Practical deployment of TPV technologies requires high power conversion efficiency (PCE) with high aesthetic quality including high average visible transmittance (AVT) and color rendering index (CRI), which can be simultaneously achieved by preferentially harvesting the ultraviolet (UV) and near-infrared (NIR) parts of the solar spectrum. [1,6] Therefore, it is beneficial to simultaneously fine-tune the absorption cutoff edges precisely at the UV/visible (VIS) and VIS/NIR borders to maximize the visible transmission (435-675 nm). [1,3,4] In the past 5 years, efforts have been made to achieve high PCE and visible transparency in TPVs. For example, the bandgaps of organometallic halide perovskite materials were sensitively tuned by compositional engineering for UV-selective-harvesting TPVs; [7,8] a series of novel low-bandgap polymer donors and non-fullerene acceptors have been applied in organic PV devices, [9,10] and excellent photovoltaic performance with distinct NIR selectivity has been demonstrated; [7,9,11-14] tandem architectures have also been utilized in TPVs to selectively harvest both UV and NIR portion of the incident solar spectrum, substantially reducing thermal losses and improving the output photovoltaic performance despite limitations imposed by current-voltage matching; [7,12] the utilization of optical outcoupling layers for VIS photons and various types of transparent electrodes can simultaneously enhance the visible transparency and the utilization of invisible photons. [11] Currently, the PCE of thin-film TPVs have reached ≈8-10%, however, the highest reported AVT is around 40-50% due to considerable parasitic absorption from the electrodes, active layers, and non-ideal wavelength-selectivity. [11,12,15] Alternatively, transparent luminescent solar concentrators (TLSCs) optically shift the solar energy conversion to edgemounted traditional PV cells via waveguided photoluminescence (PL) and total internal reflection. Without the presence of electrodes and device patterning, the structural simplicity substantially improves the defect tolerance and enables TLSCs with distinct wavelength-selectivity to achieve the highest possible visible transparency, circumventing several of the challenges for thin-film TPVs and simplifying the manufacturing. [1,3,5] Much of the previous work on TLSCs with NIR harvesting have absorption profiles that have limited UV capture with PCEs up to around 1% and AVTs above 70% for a light utilization efficiency (LUE, equal to PCE × AVT, which is introduced Visibly transparent luminescent solar concentrators (TLSC) can optimize both power production and visible transparency by selectively harvesting the invisible portion of the solar spectrum. Since the primary applications of TLSCs include building envelopes, greenhouses, automobiles, signage, and mobile electronics, maintaining aesthetics and functionalities is as important as achieving high power conversion efficiencies (PCEs) in practical deployment. In this work, massive-downshifting phosphorescent nanoclusters and ...