A new strategy has been well designed to form upended taper-shaped cuprous thiocyanate ( hereafter abbreviated as CuCNS) arrays on a copper substrate with use of a simple solution-phase method at room temperature. This method consists of a liquid-solid reaction between a solution of thiocyanate ammonium and the copper substrate itself in the assistance of formamide. Novel CuCNS arrays are approximately perpendicular to copper substrate surfaces. Every single crystal shows an upended taper-like morphology (i.e., the tip end points into the surface of copper substrate and the other big end of the taper exposes out, like a dart thrusting into the copper substrate). On the basis of structure and chemical bond analysis, CuCNS crystals tend to grow along the c-axis, which is essential for the formation of CuCNS arrays on a copper substrate. This approach also provides a facile strategy to produce different patterns on different copper substrates, which may be applicable to the synthesis of other inorganic materials with various potential applications.