Luminescent solar concentrators (LSCs) based on high photoluminescence quantum yield (PLQY) quasi-2D perovskites demonstrate superior edge light collection capability, which breaks the etendue limit and achieves signal reception in visible light communication (VLC). Herein, 2,7-bis(diphenylphosphoryl)-9,9-spirobifluorene (SPPO13) is introduced into the Q-2D RP-phase perovskite (BA(2)Cs(4)Pb(5)Br(16), <n> = 5), realizing dual effects of defect passivation and small n value phase suppression. The emission peak of the optimized film is at 518 nm with a maximum PLQY of 99.49%, and it shows excellent air storage and UV stability. The Q-2D perovskite LSCs realize an external optical efficiency of 4.3% under a geometric factor G of 3.75 and are applied to VLC systems for the first time. As a result, the VLC systems achieve an FoV exceeding +/- 30 degrees and a bandwidth of 165 MHz (-20 dB), enabling a light communication rate of 432 Mbps. This work expands the interdisciplinary application of Q-2D perovskite LSCs in VLC systems, liberating VLC receivers from complex active pointing and tracking systems.