With the rapid development of solid-state lighting and the congestion of radio-frequency communication data traffic, visible-light communication (VLC) has emerged as a versatile technology for simultaneous illumination and communication. However, the conventional color-converting phosphors integrated with light-emitting diodes (LEDs), or laser diodes (LDs) usually have limited optical modulation bandwidth due to the long carrier recombination lifetime, which is not suitable for high-speed multiple-wavelength data transfer based on phosphor-conversion VLC systems. Herein, we demonstrate a hybrid organic-inorganic perovskite nanosheets (NSs), i.e., (C <sub xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">8</sub> N <sub xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">9</sub> NH <sub xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">3</sub> ) <sub xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">2</sub> PbI <sub xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink">4</sub> (PEPI), passivated by polymer, as a fast-acting color-converting phosphor for VLC. Compared to the PEPI micro-plates ( <inline-formula xmlns:mml="http://www.w3.org/1998/Math/MathML" xmlns:xlink="http://www.w3.org/1999/xlink"> <tex-math notation="LaTeX">$\mu $ </tex-math></inline-formula> Ps), the NSs exhibit a stronger excitonic effect with a shorter fluorescence lifetime of 877 ± 4.7 ps, leading to a broad −3-dB bandwidth of 192.8 MHz. Given the large bandwidth, a net data rate of 0.93 Gb/s was achieved based on an orthogonal frequency-division multiplexing (OFDM) modulation scheme. These investigations verified the feasibility of using two-dimensional hybrid organic-inorganic perovskite materials as a promising phosphor for future multi-Gb/s color-pure wavelength-division multiplexing systems.