Chiral metasurfaces exploit structural asymmetry to control circular polarized light, presenting new possibilities for the design of optical devices, specifically in the dynamic control of light and enhanced optical sensing fields. This study employed theoretical and computational methods to examine the chiroptical properties of a bilayer crescent chiral metasurface, demonstrating the effect of the angle of rotation on the chiroptical response. We particularly investigated the changes in transmittance, electric field distribution, and circular dichroism (CD) across various rotation angles. The crescent chiral metasurface demonstrated the maximum CD and showed significant control over the CD and electric field distribution across different rotation angles in the near-infrared region. The highest CD value was observed at a 23° rotation angle, where the chiroptical response reached its maximum. In addition, the left circular polarized light showed a stronger intensity of the electric field along the crescent metasurface edge relative to the right circular polarized light, underscoring the significant difference in the intensity and field localization. It was also shown that the configuration with a 2 by 2-unit cell, compared with a single-unit cell, exhibited significantly enhanced CD, thus underlining the importance of the unit cell arrangement in optimizing the chiroptical properties of metasurfaces for advanced photonic applications. These results prove that the 2 by 2 bilayer crescent chiral metasurface can be tailored to a fine degree for specific applications such as improved biosensing, enhanced optical communications, and precise polarization control by optimizing the configuration. The insight presented by this theoretical and computational study will contribute to the broad understanding of chiroptical phenomena as well as pave the way for potential applications in developing advanced optical devices with tuned chiroptical interactions.