Nanoaggregates such as nanowires, nanoparticles, nanotubules, and nanoribbons were prepared from bulk crystals, which are shaped as needles (1), blocks (2), tubules (3 alpha), and plates (3 beta), respectively, by grinding and ultra-sonication. Nanowires have diameters of approximately 2 nm, lengths of thousands of nanmeters, and the distance between adjacent nanowires is approximately 2 nm. The diameters of nanopartides range from 3 to 5 nm. Nanotubules display diameters of 70 rim and lengths of thousands of nanometers, and nanoribbons exhibit widths of approximately 50 nm and lengths of hundreds of nanometers. All of the bulk crystals have been synthesized by the wet chemical method. Single-crystal X-ray diffraction reveals that crystal 1 is constituted by infinite one-dimensional {[NH3CH2CH(NH2)CH3](C6H4O2)[mu(2)-OC6H4O] (Mo-VI-O-Na-O)[NH2CH2CH(NH2)CH3]}(n) (1), which acts as a parallel aligned quantum wire forming lamellas that assemble themselves into multilayered architecture. Crystal 2 consists of discrete [NH3CH2CH(NH2)CH3](2)[(MoO2)-O-VI(O2C6H4)(2)] (2), which presents as quantum particles and repeats itself along a three-dimensional crystal lattice. Crystal 3a, formed under 5 C, and 3 beta, crystallized above 10 degrees C, are both composed of (NH3CH2CH2NH2)(2)[(MoO2)-O-VI(O2C6H4)(2)](NH2CH2CH2NH2)(0.5) (3) but are packed in different ways. In crystal 3 alpha, four [(MoO2)-O-VI(O2C6H4)(2)](2-) circle into a quantum tube that is further assembled into multitubular architecture. However, in crystal 3 beta two [(MoO2)-O-VI(O2C6H4)(2)](2-) form a bilayered quantum lamellar motif that is piled into multilayered architecture. TEM reveals that all of the morphologies of the nanoaggregates are associated with the structures of the quantum motifs in their crystal lattices, which provide successful and effective access to assemble controlled nanostructures from quantum motifs of fine-desired and well-ordered bulk crystals. The technology of grinding and ultrasonication to prepare nanoaggregates is simple and available.