Natrolemoynite is a new member of the lemoynite group found in altered or unaltered pegmatites cutting nepheline syenite at the Poudrette quarry, Mont Saint-Hilaire, Quebec. In altered pegmatites, it is associated with microcline, lemoynite, lepidocrocite, galena, sphalerite, calcite and pyrite, and in unaltered pegmatites, with biotite, microcline, albite, magnetite, a chlorite-group mineral, a burbankite-group mineral, an unidentified donnayite-(Y)-like mineral, zircon and pyrochlore. Crystals are colorless to white (occasionally with a slightly pink to red tinge), bladed to prismatic, elongate along [001], with maximum widths of 1 mm and lengths of 2 mm. The mineral typically develops in compact radial aggregates and spheres 4 mm in maximum diameter. It is transparent to translucent, with a vitreous to subadamantine luster and a white streak. The Mohs hardness is 3. Perfect {100} and {010} cleavages and a poor {001} cleavage are observed. D meas is 2.47(1) g/cm 3 and D calc , 2.50 g/cm 3. Natrolemoynite is biaxial negative, ␣ 1.533(1),  1.559(1), ␥ 1.567(1), 2V meas. = 63(1)°, 2V calc. = 57(1)°; dispersion is weak, with r and v crossed. The optical orientation is X = b, Z ٙ a = 41° (measured in the obtuse angle ). The average result of nineteen electron-microprobe analyses gave Na 2 O 7.47, K 2 O 1.29, CaO 0.37, MnO 0.12, Al 2 O 3 0.04, SiO 2 54.51, TiO 2 0.38, ZrO 2 21.97, Nb 2 O 5 1.01 and H 2 O (calc.) 14.72, total 101.88 wt.%, corresponding to (Na 2.66 K 0.30 Ca 0.07 Mn 0.02) ⌺3.05 (Zr 1.96 Nb 0.08 Ti 0.05) ⌺2.09 (Si 9.99 Al 0.01) ⌺10 O 25.79 • 9H 2 O on the basis of 10(Si + Al) or, ideally, Na 4 Zr 2 Si 10 O 26 •9H 2 O. It is monoclinic, C2/m, a 10.5150(2), b 16.2534(4), c 9.1029(3) Å,  105.462(2)°, V 1499.4(1) Å 3 , Z = 2. The structure was refined to R = 4.2% for 2133 reflections [F o > 4(F o)]. Six-membered rings of SiO 4 tetrahedra are linked along [001] by ZrO 6 octahedra to form a zirconosilicate framework. Channels parallel to [001] are occupied by Na and H 2 O. Evidence is provided for limited Na ↔ H 3 O + substitution. Crystal-chemical and field relations indicate that paragenetically, natrolemoynite is one of the last sodium zirconosilicate hydrate phases to develop.