The purpose of this chapter is to give a critical review of the processes involved in the generation of nanoparticles by material ablation with two time-delayed laser pulses. Experimental investigations of the ablation characteristics during nanoparticle synthesis with short double pulses are presented. In particular, the composition and the expansion dynamics of the ablated material are examined. The latest progress achieved in modeling laser-matter interactions in double pulse regime is discussed. The correlation between ablation efficiency and nanoparticle generation is assessed and compared with numerical simulations, the influence of interpulse delay on metals ablation being revealed.