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Molybdenum disulfide (MoS2), a promising two‐dimensional photothermal material, possesses the capability to convert solar irradiation into thermal energy. This conversion is beneficial for processes like wastewater treatment and seawater desalination. Nevertheless, the influence of the surface chemical properties of MoS2, particularly its wettability, on the evaporation rate of water confined to the surface remains unexplored. In our study, we demonstrate that the wettability degree of MoS2 significantly influences its water evaporation rate performance. Interestingly, this parameter can be simply and accurately modulated by altering the synthesis time of MoS2. We synthesized MoS2 via a simple hydrothermal method at three different durations: 16, 20, and 24 h, at 200°C. Subsequently, we impregnated the resultant MoS2 onto air‐laid paper (ALP), forming a solar‐driven evaporator system. We found that the MoS2 nanosheets synthesized within the shortest duration (MoS2‐16 h) exhibited the highest evaporation rate of 1.77 kg m−2 h−1, along with 92% energy efficiency. MoS2‐16 h resulted in MoS2 rich in defects, featuring the largest surface area and the smallest contact angle. The hydrophilic areas of MoS2‐16 h facilitated the continuous diffusion of water molecules through defect sites, treating them as contact lines. Additionally, the expansive surface area introduced a larger region for light absorption, enhancing water‐solid interactions. The presence of molybdenum oxide on the surface of the nanosheet system also contributed to superior wettability behavior. Notably, all the tested MoS2/ALP systems in this study displayed excellent performance in salt rejection and heavy metal ion concentration reduction.