On the basis of the highly oriented ZnO nanoparticle nanoribbons as the growth seed layer (GSL) and solution growth technique, we have synthesized vertical ZnO nanorod arrays with high density over a large area and multi-teeth brush nanostructure, respectively, according to the density degree of the arrangement of nanoparticle nanoribbons GSL on the glass substrate. This controllable and convenient technique opens the possibility of creating nanostructured film for industrial fabrication and may represent a facile way to get similar structures of other compounds by using highly oriented GSL to promote the vertical arrays growth. The growth mechanism of the formation of the ordered nanorod arrays is also discussed. The second-order nonlinear optical coefficient d 31 of the vertical ZnO nanorod arrays measured by the Maker fringes technique is 11.3 times as large as that of d 36 KH 2PO 4 (KDP).