The first column of two-dimensional (2D)-layered metal-complex-templated nickel borate was obtained by using a solvothermal synthesis method. The 2D nickel borate [Ni(en)(3)]center dot[Ni0.5B6O8(OH)(4)]center dot Cl (1; en = ethylenediamine) contains [Ni(en)(3)](2+), Cl-, and the first reported inorganic nickel borate layer [Ni0.5B6O8(OH)(4)](-), which is formed by the interconnection of Ni and O atoms in the B-O cluster. By increasing the reaction temperature during the synthesis process of compound 1, the one-dimensional (1D) chain nickel borate [Ni(en)(3)](2)center dot[B7O10(OH)(3)]center dot Cl-2 (2) was obtained, wherein the [B7O10(OH)(3)] cluster was connected through an O atom to form a ID chain structure. By adjusting the molar ratio of the raw materials, that is, adjusting the pH of the reaction, the other 1D chain nickel borate Ni(en)(3)center dot Hen center dot[B9O13(OH)(4)]center dot H2O (3) was obtained, in which [B5O8(OH)(2)] and [B4O7(OH)(2)] clusters can be connected via a common O atom to form an infinite [B9O13(OH)(4)] polyanionic chain. Meanwhile, we successfully synthesized the isoform of compound 3 with the metal cadmium.