Harvesting atmospheric water and converting it into electricity play vital roles in advancing next-generation energy conversion systems. However, the current water harvester systems suffer from a weak water capture ability and poor recyclability due to high diffusion barriers and low sorption kinetics, which significantly limit their practical application. Herein, we drew inspiration from the natural "Pump effect" observed in wood and successfully developed a dual "absorption−adsorption" networked MXene aerogel atmospheric water harvester (MAWH) through ice templating and confining LiCl processes, thereby serving multiple purposes of clean water production, passive dehumidification, and power generation. The MAWH benefits from the dual H-bond network of MXene and cellulose nanocrystals (absorption network) and the hygroscopic properties of lithium chloride (adsorption network). Furthermore, its aligned wood-like channel structure efficiently eliminates water nucleation near the 3D network, resulting in fast moisture absorption. The developed MAWH demonstrates a high moisture absorption ability of 3.12 g g −1 at 90% relative humidity (RH), featuring rapid vapor transport rates and durable cyclic performance. When compared with commercial desiccants such as the 4A molecular sieve and silica gel, the MAWH can reduce the RH from 80% to 20% within just 6 h. Most notably, our integrated MAWH-based water harvesting−power generation system achieves a high voltage of ∼0.12 V at 77% RH, showcasing its potential for practical application. These developed MAWHs are considered as high-performance atmospheric water harvesters in the water collection and power generation field.