The strong absorption of light [ 1 ] and the local amplifi cation of the electromagnetic fi eld [ 2 ] at the plasmon resonance of noble metal nanostructures have been the focus of hundreds of studies due to their practical applications for the fabrication of optical devices such as fi lters, non-linear optical components, or Raman enhancers. [ 3,4 ] The control of the plasmon features such as spectral width, [ 5 ] position, [ 6 ] and shape [ 7 ] can be accomplished by different physical deposition routes [8][9][10][11][12] providing adequate growing conditions of metal nanoparticles (MNPs). Pioneer works in the 1990s showed the optical selectivity of elongated Ag deposits on SiO 2 with applications as optical fi lters for windows to control solar heat gain and glare, among others. [ 13 ] Recently, assemblies of parallel stripes of MNPs have been fabricated onto preformed surfaces presenting a 1D periodic roughness [ 14 , 15 ] or bundled SiO 2 nanocolumns. [ 16 , 17 ] A signifi cant macroscopic optical dichroism has been reported for these systems that can be useful for the development of polarized light emitters or materials with an enhanced IR luminescence because of the excitation of two distinct plasmon resonances in the directions parallel (longitudinal mode) and perpendicular (transverse mode) to the stripes. [ 18 ] Architecture control of the metal assemblies plays a determinant role in the functional properties of the material. For this purpose, the softlithographic techniques provide means to accurately tailor the nanostructure of the materials. [18][19][20][21] Laser scanning is a softlithographic technique widely used to modify the shape and structure of metal nanoparticles. [21][22][23][24] Surface modifi cation can be easily achieved by in situ [ 21 ] or ex situ [22][23][24] pulsed laser treatment in the case of random systems of MNPs. In contrast, nothing has been reported about the effect of a pulsed laser on the structure and optical dichroism of autoorganized metal nanostructures. In this paper we show that nanosecond (ns) laser irradiation can be effectively used to control the optical dichroism of Ag stripes supported on SiO 2 nanocolumns (NCs). This dichroism can be effectively tailored along the full visible range. Thus, we propose the utilization of the AgNPs/SiO 2 NCs structures for writing dichroic patterns at the microscale with potential applications for encryption and data storage purposes.AgNPs/SiO 2 NCs fi lms were grown by a two-step process.[ 17 ]First, SiO 2 thin fi lms were deposited by glancing angle vapor deposition (GLAD) with a tilted columnar nanostructure and ≈ 350 nm thickness (see Figure S1a in the Supporting Information and the Experimental Section). [ 25 , 26 ] These structures present an anisotropic surface topography known as "bundling", [ 17 ] consisting of the coalescence of the NCs along the x -direction ( Figure S1b). The silver nanoparticles were then grown by DC sputtering at room temperature. The "bundled" SiO 2 NCs act as a template for the fabrication of Ag...