Lighter-than-air (LTA) vehicles like aerostats and airships are increasingly favored for high-altitude surveillance and communication missions. These vehicles employ a fabric enclosure filled with helium for lift, enabling efficient payload transport to predetermined heights. Impermeable coated or laminated inflatable textile structures have been established as lightweight composite assemblies for LTA systems. The critical risk factors in their development include envelope strength, gas barrier, and weather resistance. Degradation of the inflatable envelope due to severe weathering stresses like temperature, UV radiation, and rain can significantly reduce its barrier properties, limiting its service life and causing financial loss. Optimization of properties and functional improvements are crucial. This paper critically reviews global research on the technology and materials for aerostats and airships, providing an overview of their structures and envelope material development. Strategies for gas barrier and weathering resistance are examined, along with the potential of advanced polymer nanocomposites as envelope materials.