Recently, the optical properties of silicon (Si) submicrometer spherical particles have been investigated to understand the dielectric nano-photonic function. Herein, we fabricated Si submicrometer spherical particles with high scattering efficiency using pulsed laser melting in deionized water or ethanol by irradiating laser at 66 mJ pulse-1 cm-2 via third harmonic of Nd:YAG laser. Hydrofluoric acid pretreatment was effective to remove surface oxide of raw Si particles; the laser fluence to obtain well crystallized spherical particles was lowered to 20 mJ pulse-1 cm-2 and the crystallinity of particles obtained were greatly improved without forming unwanted byproducts. The amount of particles was much more than those obtained by conventional fabrication technique. The particle size can be controlled by changing the laser fluence, and the scattering wavelength of colloidal solution can be controlled from visible to the near infrared range by increasing the laser fluence.