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Amidst the rapid advancements in the fields of photovoltaics and optoelectronic devices, CsPbBr₃ nanosheets (NSs) have emerged as a focal point of research due to their exceptional optical and electronic properties. This work explores the application potential of CsPbBr₃ NSs in photonic and catalytic domains. Utilizing an optimized hot-injection method and a ZnBr₂-assisted in situ passivation strategy, we successfully synthesized CsPbBr₃ NSs with controlled dimensions and optical characteristics. Comprehensive characterization revealed that the nucleation environment and thickness significantly influenced the structure and optical performance of the materials. The results indicate that the optimized synthesis method enables control over the lateral dimensions of the nanoparticles, ranging from 9.1 ± 0.06 nm to 334.5 ± 4.40 nm, facilitating the tuning of the excitation wavelength from 460 nm (blue) to 510 nm (green). Further analyses involving photoresponse and electrochemical impedance spectroscopy demonstrated the substantial potential of these NSs in applications such as photocatalysis and energy conversion.