Semiconductor photocatalysts play a pivotal role in fostering a sustainable environment by harnessing solar energy directly into chemical energy to achieve various photocatalytic processes. Therefore, a visible-infrared active photocatalyst is the next level of demand for solving the alarming environmental issues. In this regard, the present article reports the investigations of crucial mechanisms and conditions leading to pure and defect-free hexagonal 2D CuSe nanosheets (NSs) and the influence of their structural architecture on visible-infrared active photocatalytic performance. Here, it was achieved by the conventional hydrothermal method by varying the pH of the reaction mixture. XRD analysis was used to examine the crystal structure and lattice parameters of CuSe NSs. The presence of H+ ions was suggested to significantly influence the observed anisotropic crystallite growth across different pH conditions. EDS and XPS analysis exhibited the purity and stoichiometry of 2D CuSe NSs, revealing that the obtained stoichiometry was consistent with CuSe composition. The morphological characteristics were investigated using FE-SEM as well as HR-TEM analyses, and the specific surface area was determined using Brunauer-Emmett-Teller analysis in which a significant change occurred in response to the variation in reaction conditions. The optical properties of optimized 2D CuSe NSs show excellent absorption in the visible and near-infrared region utilizing full solar with a notable decrease in emission intensity, suggesting a reduction in recombination rates due to pH-induced changes in the nanoarchitecture. Herein, methylene blue, a well-established model dye, was used as a probe to assess the photocatalytic activity of the synthesized CuSe NSs. Notably, the CuSe NSs synthesized under neutral conditions demonstrate a remarkable methylene blue degradation efficiency, reaching approximately 98 % within approximately 45 minutes, indicating a high degradation rate. Finally, an in-depth exploration into the intricacies of photocatalytic performance, degradation mechanisms, and the recyclability test was conducted, accompanied by a thorough investigation into the feasibility of CuSe NSs for their practical application in photocatalytic wastewater treatment.