the architectural envelope as they become more scalable, converting new and existing infrastructure into power-generating sources and dramatically reducing the electrical loss in transmission. [4,5] Transparent luminescent solar concentrators (TLSCs), a key TPV technology, optically shift the solar energy conversion by photoluminescence (PL) that is transported optically (by total internal reflection) to edge-mounted PV cells ( Figure 1A). [1] Due to the absence of electrodes, busbars, and collection grids over the solar harvesting area, the device structure is largely simplified, which enables LSC/TLSC devices to achieve the highest levels of transparency and aesthetics. [4,5] In the past decade, quantum dots, [6][7][8] nanoclusters, [9] and rare-earth ion complexes [10][11][12][13] have been widely investigated as the luminophores in LSC/TLSC systems. Most of these works focus on 1) the improvement of quantum yield (QY), [5,14,15] 2) the modulation of the absorption and emission spectra to minimize the reabsorption loss, [7,8,10,16] and 3) the enhancement of light absorption by matching the absorption spectrum of the luminophores with the peak of the incident solar spectrum. [17][18][19][20] However, the continuous-band absorption characteristics of these luminophores limit their absorption cut-off to ≈435 nm, if a high aesthetic quality and transparency is targeted. Bandgaps beyond 440 nm can result in rapid drops in average visible transmittance (AVT) and color rendering index (CRI). [1,2,21] Utilizing wavelength selective absorbers makes it possible to harvest just the UV or NIR. As selective absorption redshifts beyond 675 nm, the CRI and AVT reach a maximum. [1,2] Therefore, NIR photons between 675 nm and the absorption cut-off of the edge-mounted PV cell can be utilized for power generation, and this range coincides with the peak of the incident AM 1.5G photon flux. Moreover, even with tail absorption in the red-NIR below 675 nm, the resulting blue/green tint is often more visually acceptable than yellow/red tinting, which offers more design freedom for NIR selective-harvesting luminophores. [1,2,22] Optical absorption in organic and molecular semiconductors originates from the transition from the ground state to excited molecular orbitals (e.g., S 0 → S 1 , S 0 → S 2 ). The gap between the excited molecular orbitals (S 1 and S 2 ) results in discontinuity in the density of states, which allows the transmission of photons. The molecular structure can be designed so that this gap is Transparent luminescent solar concentrators (TLSCs) selectively harvest ultraviolet and near-infrared photons. Due to the absence of electrodes, busbars, and collection grids over the solar harvesting area, the device structure enables these devices to achieve the highest levels of transparency and aesthetics. Recently, CO i 8DFIC has been developed as a nonfullerene acceptor in organic photovoltaics with unprecedented performance. In this work, nonfullerene acceptors are introduced into TLSCs as the luminophores. The impact of...