Metal-organic frameworks (MOFs) for sorption-based atmospheric water harvesting (AWH) are promising for solving the global water crisis, but there are two major challenges: scaled-up production and high-performance modular device design. Herein, we propose a comprehensive solution encompassing large-scale synthesis coupled with an ultra-dense modular solar-driven device without auxiliary equipment. In our study, 0.1 kg Ni2Cl2(BTDD) per batch was achieved by reflux synthesis, with a yield of 84% and a space-time yield of 630 kgMOF m−3 month−1. Benefiting from this, we realized the application of this efficient physisorbent at device level. We analyzed the AWH process to obtain thermal requirements on two scales: the entire device and each component. After the optimization on both scales, the proposed device with an integrated modular design showed ultra-high water harvesting per unit volume of 23 L m−3 and water yield up to 840.5 g m−2 under 1 sun in 7 h.