A reinvestigation of the structure of acetylcholine bromide, [CTHI602N]+Br -, with X-ray diffraction intensities collected from two untwinned crystals has been carried out. The crystals are monoclinic, space group P21/n, with a= 10.966 (4), b= 13.729 (7), c=7-159 (4)/l, fl= 108.18 (7) °, Z=4. The structure was refined by full-matrix least-squares calculations with 1730 observed reflexions, and anisotropic temperature factors for all non-hydrogen atoms. The final R was 0.041. Atomic coordinates, thermal parameters, bond lengths and angles are compared with those from previous work on acetylcholine derivatives.