Coordination polymers are among the most favored active materials by researchers due to their broad application prospects. However, most of them are usually difficult to directly process into applicable devices because of their unsatisfied processability. One process of great concern for researchers is the in situ preparation of the coordination polymer on the applicable substrate, especially for the favored network substrates with good mechanical properties and 3D porous structure, which could provide obvious convenience and facilitation in the application process. Herein, we present an ultrafast and scalable thermal current-induced dewetting strategy to obtain uniform coordination polymer film in situ on network substrates, which could enable unprecedented convenience to obtain directly usable coordination polymer composites such as practical catalytic electrodes with excellent electrocatalytic performance. The proposed thermal current-induced dewetting method provides a highly adaptable and efficient practical production approach to integrate coordination polymer materials with network substrates and also provides new inspiration for understanding and applying the dewetting process on complex 3D network substrates.