Carbon nanoparticle appearing in perfect spherical shape, with sizes varying from tens nanometers to several micrometers, can be produced by pulsed-laser ablating different elementary carbon samples immersed in water. A variety of samples including HOPG,graphite, arcdischarging deposite, glassy-carbon and imitation-diamond have been tried.The yield of the diamand nanospherulite is found to depend on the structure of the sample.The SAED pattern of the carbon-sphere produced from arc-discharging deposite can be at-tributed to the hexagonal structure of diamond, and its HREM image exihibits 0.38nm×0.31 nm lattice, which is just three times of the distances for (110) (d=0.126 nm) and (004) (d=0.1030nm) crystal layers of hexagonal diamond, respectively. While the SAED pattern from glassy-carbon sample displays a cubic-diamond structure. Furthermore, Raman spectra and 13C NMR indicate tetrahedral network of the spheres.