Near infrared ultrafast pulsed laser is used to ablate pure metal and metal alloy targets in a vacuum chamber. We find that by optimizing the ablation conditions, as a direct result of ultrafast laser ablation, crystalline nanoparticles can be abundantly produced without intermediate nucleation and growth processes. Combining with different background gases, versatile structural forms can also be obtained for the nanocrystals. Using metal nickel as a sample material, we have produced Ni/NiO core/shell nanospheres and NiO nanocubes. We also study the production of alloy nanoparticles, which has been challenging in fabrication. We demonstrate production of nanoparticles containing up to three metal elements using ultrafast laser ablation. The laser ablation process is investigated using an ion probe in real-time. Nanoparticle samples are examined using atomic force microscopy and high resolution transmission electron microscopy for morphological, structural, and chemical analysis. This study provides a simple physical method for generating nanoparticles with a narrow particle size distribution, a high particle yield, versatile chemical compositions and structural forms.