A drying environment is always a proposition faced by dynamic living organisms using water, which are driven by biopolymer-based micro- and macroanuctures. Here, we introduce a drying process for aqueous liquid crystalline (LC) solutions composed of biopolyrner with extremely high molecular weight components such as polysaccharides, cytoskeletal proteins, and DNA. On controlling the mobility of the LC microdomain, the solutions showed milliscale self integration starting from the unstable gas-LC interface during drying. In particular, we first identified giant rod-like microdomains (similar to 1 mu m diameter and more than 20 mu m length) of the mega-molecular polysaccharide, sacran, which is remarkably larger than other polysaccharides. These microdomains led to the formation of a single milliscale macrodomain, on the interface. In addition, the dried polymer films on a solid substrate also revealed that such integration depends on the size of the microdomain. We envision that this simple drying method will be useful not only for understanding the biopolymer hierarchization at the mactoscale level but also for preparation of surfaces with direction controllability, as seen in living organisms, for use in various fields such as diffusion, mechanics, and photonics.