The dispersion properties of single-walled aluminosilicate nanotube (AlSiNT) and double-walled aluminogermanate nanotube (AlGeNT) in aqueous media of poly(vinyl alcohol) (PVA) are systematically revealed using (polarized/depolarized) dynamic light scattering, rheological, rheo-optical, and scanning electron microscopy analysis schemes. The nanotube/polymer dispersions under investigation show excellent nanotube dispersion in aqueous media, and their optical transparency greatly facilitates a systematic exploration of structural features along with rheological and rheo-optical properties. The AlSiNT/PVA dispersions exhibit critical gel-like feature, providing the essential fluid elasticity for producing uniform and defect-free electrospun fibers. Similar features were noted for AlGeNT/PVA dispersions, with generally fewer nanotube loading. Additionally, there is the first evidence of liquid crystal-like “wagging” behavior for the nanotubes under steady shearing, as resolved by flow-birefringence measurement. Overall, there seems to be a potential wide range of nanotechnological applications with this particular class of nanotube/polymer aqueous dispersions.