A novel synthesis method of fibrillar trimolybdates with the use of Ag 2 Mo 3 O 10 ∙2H 2 O as a precursor has been used successfully to synthesize methylammonium trimolybdate, (CH 3 NH 3 ) 2 Mo 3 O 10 ∙H 2 O. The crystal structure of this compound was determined by X-ray powder diffraction method and refined by the Rietveld method. The compound is orthorhombic, space group P n m a (62), with a =11.241(3), b =7.585(1), and c =15.516(4) Å. The redetermined crystal structure of the precursor and the structure of the title compound are compared and discussed.