The preparation of nanocomposite structures consisting of polymers and metallic nanoparticles is of considerable interest for a variety of functional applications [1]. However, the unique properties of these nanomaterials are largely governed by the size, shape and configurations of the nano-clusters distributed in a matrix. For this reason, different preparation methods were introduced with the attempt to change and control the form and structure of such nanoparticle assemblies. Besides typical wet-chemical approaches [2, 3], polymer-metal nanocomposites were prepared by the thermal evaporation of metals on polymer substrates [4], metal-ion implantation in polymers [5], and the simultaneous plasma polymerization and metal evaporation methods [6]. In this study we prepared the gold-polymer nanocomposites using the pulsed laser deposition (PLD) technique.So far, a number of materials have been used as substrates for the PLD of noble metals including metal oxides [7], silicon or glass substrates [8][9][10], and polymers [8,11,12]. Typically, at lower values of volume concentration of the metallic phase in the matrix, the PLD produces well separated particles with narrow size distributions. However, at higher amounts of deposited material the proximity of the nanoparticles leads to their coalescence, which impairs the control of particle sizes inherent to PLD. To address this problem several methods were suggested. For example, Röder and Krebs [11] used the pre-deposition of more reactive metals that act as nucleation centers for the nanoparticle growth, while Resta et al. [13] sharpened the shape distribution of metal nanoparticles using laser irradiation. Here we show that the dense packing of gold nanoparticles can be achieved in a simple manner if a blend of the amino-terminated polystyrene (PS-NH 2 ) and carboxylterminated polymethylmethacrylate (PMMA-COOH) is used as a PLD substrate. It should be emphasized that the preparation of this type of nanostructures with densely packed, monodispersed, and supported metallic nanoparticles is of importance for a number of applications such as surface enhanced vibrational spectroscopy substrates [9] or I -V switches [14].PS-NH 2 (M n = 29 000 g/mol, PD = 1.4) and PMMA-COOH (M n = 26 800 g/mol, PD = 1.18) have been synthesized by ATRP [15] and RAFT [16], respectively. 15 µm thick films of the pure PS, PS-NH 2 , PMMA-COOH or of the (PS-NH 2 + PMMA-COOH) blend (1 :1 by weight) used for the Au deposition were prepared by solution casting on Densely packed gold nanoparticles with narrow size distribution were fabricated by pulsed laser deposition using a blend of amino-terminated polystyrene (PS-NH 2 ) and carboxylterminated polymethylmethacrylate (PMMA-COOH) as a deposition substrate. Transmission electron microscopy showed spherical Au nanoparticles with an average size of 5 nm. UV-vis absorption spectra of the Au/blend nanocomposite films exhibited a strong resonance band at 658 nm. The analyses of the spectrum using the effective medium Bergman theory showed that the nano...