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Summary Colloidal quantum dots (QDs) are promising building blocks for luminescent solar concentrators (LSCs). For their widespread use, they need to simultaneously satisfy non-toxic material content, low reabsorption, high photoluminescence quantum yield, and large-scale production. Here, copper doping of zinc carboxylate-passivated InP core and nano-engineering of ZnSe shell facilitated high in-device quantum efficiency of QDs over 80%, having well-matched spectral emission profile with the photo-response of silicon solar cells. The optimized QD-LSCs showed an optical quantum efficiency of 37% and an internal concentration factor of 4.7 for a 10 × 10-cm2 device area under solar illumination, which is comparable with the state-of-the-art LSCs based on cadmium-containing QDs and lead-containing perovskites. Synthesis of the copper-doped InP/ZnSe QDs in gram-scale and large-area deposition (3,000 cm2) onto commercial window glasses via doctor-blade technique showed their scalability for mass production. These results position InP-based QDs as a promising alternative for efficient solar energy harvesting., Graphical Abstract, Highlights • The luminescent solar concentrators based on copper-doped InP QDs are demonstrated • Efficient excitation transfer led to the exceptionally high in-film PLQY of 81.2% • The LSCs based on copper-doped QDs showed the optical quantum efficiency of 37% • The gram-scale synthesis of QDs led to the fabrication of large-area LSCs (3,000 cm2), Nanoparticles; Energy Resources; Energy Engineering; Energy Materials