Metal-organic frameworks (MOFs) are promising adsorbents for atmospheric water harvesting (AWH), particularly in arid climates. However, the inherently narrow pores (typically with sizes < 2 nm) of conventional MOFs limit both water diffusion and adsorption capacity, thereby constraining the practical daily water yield of MOF-based AWH systems. Herein, ordered mesopore engineering is applied to a typical hygroscopic MOF, UiO-66-NH2, to construct channels with larger pores, thereby overcoming these limitations. The resulting material with uniform 11 nm 2D hexagonal mesopores, denoted OM-UiO-66-NH2, exhibits a 3.7-fold faster water adsorption rate and nearly an order-of-magnitude higher effective water diffusivity than the pristine UiO-66-NH2 at 30% relative humidity (RH). Moreover, OM-UiO-66-NH2 achieves a 12% increase in water uptake capacity (0.43 g g(-1) at 30% RH) and maintains stable performance over 500 adsorption-desorption cycles. When integrated into a modular harvester, OM-UiO-66-NH2 exhibits ultrafast adsorption (92% saturation within 5 min) and high condensation efficiency (94%), achieving a daily water yield of 27.8 L kg(-1) day(-1) at 30% RH. This study demonstrates that ordered mesopore engineering effectively overcomes diffusion limitations in MOFs, advancing the design of high-performance materials for efficient AWH in arid environments.