Dense layers of overlapping three-dimensional (3D) gold nanodendrites characterized by high specific surfaces as well as by abundance of sharp edges and vertices creating high densities of SERS hotspots are promising substrates for SERS-based sensing and catalysis. We have evaluated to what extent structural features of 3D gold nanodendrite layers can be optimized by the initiation of 3D gold nanodendrite growth at gold particles rationally positioned on silicon wafers. For this purpose, galvanic displacement reactions yielding 3D gold nanodendrites were guided by hexagonal arrays of parent gold particles with a lattice constant of 1.5 μm obtained by solid-state dewetting of gold on topographically patterned silicon wafers. Initiation of the growth of dendritic features at the edges of the gold particles resulted in the formation of 3D gold nanodendrites while limitation of dendritic growth to the substrate plane was prevented. The regular arrangement of the parent gold particles supported the formation of dense layers of overlapping 3D gold nanodendrites that were sufficiently homogeneous within the resolution limits of Raman microscopy. Consequently, SERS mapping experiments revealed a reasonable degree of uniformity. The proposed preparation algorithm comprises only bottom-up process steps that can be carried out without the use of costly instrumentation.