Compared with traditional rain gauges and weather radars, hydrogel flexible electronic sensor capable of responding directly to rainfall events with promptness and authenticity, shows great prospects in real-time rainfall monitoring. Aluminum coordination hydrogel (Al-HG), one of the most qualified sensors suitable for rainfall monitoring, however, is currently impeded from widespread application by its weak mechanical properties due to the low binding strength between Al³⁺ and functional ligands. Herein, inspired by the antifreeze proteins (AFPs) that protect those Patagonian toothfishes by strongly binding to ice crystals at freezing temperatures, a low temperature-induced strategy is introduced to promote more and stronger ligand carboxyls firm combination with Al³⁺, thus forming a high-coordinated structure to deal with this challenge. Expectedly, the whole mechanical performance of the product Al-HG_F1/F2 obtained by the low temperature-induced strategy is improved. For example, the tensile fracture toughness and the maximum compressive stress of Al-HG_F1/F2 are 1.66 MJ·m⁻³ and 12.01 MPa, approximately twice those of the sample Al-HG_F3/F0 obtained by traditional soaking method (0.86 MJ·m⁻³ and 7.38 MPa, respectively). Coupled with its good biocompatibility, ionic conductivity, and sensing ability, Al-HG_F1/F2 demonstrates promising application for real-time rainfall monitoring in discrepant rainfall intensities, different zones, and even under extreme environments. This work aims to offer a stride toward mechanically robust aluminum coordination hydrogel sensors for real-time rainfall monitoring as well as provide insights into flood prevention and disaster mitigation.