During last decade, laser-based synthesis of nanoparticles and nanostructures has attracted particular attention [1]. Nanoparticles demonstrate unique plasmonic and/or photoluminescent properties, as well as a capacity of field amplification. These effects are essential in many promising applications, such as imaging, sensors, photodynamic therapy, etc. Many of medical applications require the absence of any toxicity and/or of the incompatibility with biological tissues. Nanoparticle and nanostructure generation by laser ablation provides possibilities to respect such strict requirements [2]. This study is aimed at the better understanding of the mechanisms involved in nanoparticle formation by laser ablation and at the possibilities of the process optimization. For this, we carry out very detailed simulation based on combined numerical methods. In particular, we focus our attention on the role of laser parameters and ambient environment in both target decomposition and following laser plume dynamics. The obtained results are also used to explain several promising experiments where nanoparticles and nanostructures are obtained with unique properties that are impossible to reproduce by other methods. [1] D. B. Geohegan et al., Appl.Phys. Lett. 72, 2987 (1998) [2] S. Besner et al., Appl. Phys. A 93, 955-959 (2008)