Three different dimensional zinc phosphites and zinc phosphates, [C7H18N]2[Zn(HPO3)2] (1), [C6H9N2][Zn2(PO4)(HPO3)] (2), and [C6H14N2][Zn2(PO4)2] (3) were hydro(solvo)thermally synthesized from organic amines with the same number of nonhydrogen atoms and different dimensionalities and sizes. Structural analysis indicates that compound 1 shows a one-dimensional (1D) chain structure; compound 2 is an inorganic–organic hybrid two-dimensional (2D) material; compound 3 is a three-dimensional (3D) open-framework zinc phosphate EDI zeolite. The mechanisms of 1D chain-like n-heptamine, 2D planar 3-aminomethylpyridine, and 3D triethylenediamine on the synthetic process were analyzed. The n-heptamine has only one function: a protonated template in compound 1, while 3-aminomethylpyridine has two functions: a protonated template and binding ligand in the synthesis of compound 2. The triethylenediamine has three functions in compound 3: a protonated template, space-filling agent, and structure-directing agent. Thus, the three organic amines play different roles in the three compounds. They were analyzed by XRD, SEM, TGA, FT-IR, ICP, and CHN analyses.