The synthesis, structure, and infrared spectroscopy properties of the new organically templated uranyl sulfate Na(phgH ⁺) ₇[(UO ₂) ₆(SO ₄) ₁₀](H ₂O) _3.5 (1), obtained at room temperature by evaporation from aqueous solution, are reported. Its structure contains unique uranyl sulfate [(UO ₂) ₆(SO ₄) ₁₀] ^8- nanotubules templated by protonated N-phenylglycine (C ₆H ₅NH ₂CH ₂COOH) ⁺. Their internal diameter is 1.4 nm. Each of the nanotubules is built from uranyl sulfate rings sharing common SO ₄ tetrahedra. The template plays an important role in the formation of the complex structure of 1. The aromatic rings are stacked parallel to each other due to the effect of π-π interaction with their side chains extending into the gaps between the nanotubules.