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Large-size luminescent solar concentrators (LSCs), which act as a complement to silicon-based photovoltaic (Si-PV) systems, still suffer from low power conversion efficiency (PCE). How to improve the performance of LSCs, especially large ones, is currently a hot research topic. Traditional LSCs have only a single transmission mode of fluorescence from the luminescent materials to the Si-PV, but here we introduce a new idea to improve the absorption of Si-PV by employing dual transmission modes of both fluorescence and scattering light. To prepare LSCs with dual mode transmission, Si-PV systems are coupled around the edges of a light-harvesting slice, which is prepared by ultraviolet light-induced polymerization of methyl methacrylate (MMA) solution containing both luminescent CsPbBr3 and TiO2 nanocrystals (NCs). When the sun light or incident light is coupled into the light-harvesting slice, CsPbBr3 NCs can convert the incident light into fluorescence, and then partly transmit to Si-PV at the edges, where the light is finally converted into electrical energy. Besides the traditional fluorescence transmission mode, the addition of TiO2 brings another transmission mode, namely the scattering of incident light to Si-PV, leading to an increase in PCE. In comparison to that of pure CsPbBr3-based LSCs without the addition of TiO2 (0.97%), the PCE of TiO2-doped LSCs with a large size of 20 cm × 20 cm is improved to 1.82%. The maximal PCE appears for LSCs with a size of 5 cm × 5 cm, reaching 2.62%. The reported method of dual transmission modes is a new alternative way to improve the performance of LSC devices, which does not need to change the optical properties of luminescent materials. Moreover, the production process is simple, low-cost and suitable for preparing large area LSCs, further promoting the application of LSCs.

As large‐area photon collection devices designed to convert sunlight into electricity, luminescent solar concentrators (LSCs) have been proposed for more than 40 years. In practical sunlight‐harvesting applications, existing glass windows or curtain walls have to be torn down and then replaced by traditional LSCs with planar optical waveguides, leading to high manufacture and installation costs. One alternative and attractive approach is to design and manufacture LSCs that are compatible with and can be attached directly onto the original building glass windows, which substantially reduces the overall costs. Herein, a feasible strategy of attachable transparent LSCs is proposed, converting ordinary glass to LSCs by simply attaching novel luminescent films. By integrating a phenylethylammonium (PEA)‐assisted perovskite−PVDF composite film with a polymer antireflection/barrier layer, as‐prepared composite films show dramatical improvement in photoluminescence quantum yield from 4.1% to 45.8% (11‐fold enhancement), substantially increased optical transmittance from 30.9% to 71.1% (at 700 nm), as well as strongly suppressed photoluminescence (PL) quenching during the attaching process. The fabricated attachable LSCs demonstrate a maximum optical efficiency of 2.8% at the geometric factor of 5 and retain 87% of initial optical efficiency after 2 months of storage in ambient conditions.