All-small-molecule dynamic hydrogels have shown great promise in cell culture, tissue engineering, and controlled drug release. The further development of more kinds of all-small-molecule dynamic hydrogels is severely hindered by the lack of enough commensurate building blocks from nature and on the market. Inspired by the widely developed metal-organic framework structures, herein we report a facile fabrication of metallogels by direct gelation of small molecular compounds including aminoglycosides (AGs), 2,2'-bipyridine-4,4'-dicarboxaldehyde (BIPY), and metal ions via coordination interactions and Schiff base reactions. These prepared metallogels exhibited good biodegradability and biosafety, excellent conductivity, tunable mechanical properties and potent antibacterial activities both in vitro and in vivo. This study provides a new strategy for expanding the scope of all-small-molecule dynamic metallogels for various biomedical applications.