The synthesis, structure, and infrared spectroscopy properties of the new organically templated uranyl sulfate Na(phgH+)7[(UO2)6(SO4)10](H2O)3.5 (1), obtained at room temperature by evaporation from aqueous solution, are reported. Its structure contains unique uranyl sulfate [(UO2)6(SO4)10]8− nanotubules templated by protonated N-phenylglycine (C6H5NH2CH2COOH)+. Their internal diameter is 1.4 nm. Each of the nanotubules is built from uranyl sulfate rings sharing common SO4 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.