The crystal−liquid−glass phase-transition behavior of coordination polymers (CPs) endows them with unique processing and mechanical properties to prepare functional CP glass films. However, their potential applications are still waiting to be explored. In this study, flawless [Zn(HPO 4 )(H 2 PO 4 ) 2 ](H 2 Im) 2 (abbreviated as ZnP-H 2 Im) glass films are facilely prepared through rapid hot casting coupled with melt quenching. Relying on the grain-boundary-free structure of the film and nonporous structure of the coordination network, undesired diffusion of guest molecules in ZnP-H 2 Im glass films can be effectively prohibited, which is advantageous for gas permeation and liquid leakage prevention. Gas permeation test results indicate that the barrier efficiency of the ZnP-H 2 Im glass film to gas molecules reaches 100%, while polarization curve and EIS results imply that prepared ZnP-H 2 Im glass film possesses excellent corrosion resistance in salt aqueous solution with a protection efficiency up to 99.98% for metallic substrate. Our research demonstrates that CP glasses hold great potential to serve as competent gas barrier layers and corrosion-resistant coatings.