The properties of (synthesized) single-walled aluminosilicate nanotube (AlSiNT; light-scattering characterized length similar to 2000 +/- 230 nm and diameter similar to 35 +/- 4 nm) dispersed in an aqueous poly(vinyl alcohol) (PVA) solution (10 wt %) are systematically explored using a comprehensive combination of (polarized/depolarized) dynamic light scattering, theological, rheo-optical, and scanning electron microscopy analysis schemes. The nanotube/polymer dispersions under investigation are promising for their fair nanotube dispersion in pristine aqueous media (e.g., without salt or acid addition), as well as for the optical transparency that greatly facilitates systematic exploration of structural features and dispersion state that are practically inaccessible for many of their (opaque) companions such as carbon nanotube dispersions. We provide the first in-depth analysis revealing excellent dispersion state of (unmodified) AlSiNT in the PVA matrix, giving rise to (critical) gel-like features and substantially promoted elasticity that can be utilized, as a practical assessment, to produce uniform and defect-free electrospun nanofibers. Additionally, there is unambiguous evidence of nematic liquid crystal- like "wagging" (strain-invariant, periodic oscillation) under steady shear flow, a phenomenon previously unreported for nanotube composite materials. Overall, the present findings suggest that AlSiNT/PVA dispersions possess promising theological, optical, and electrospinning properties that are highly desirable for current nanotechnological applications, and may serve as an ideal model system for establishing structure-performance relationships for like nanotube/polymer composite materials.