The GaxCo0.6-xZnS0.4 (x = 0.1, 0.3, 0.5) nanoparticles with shuttle-shaped are fabricated via a Magnetic Polarization Pulse Laser Ablation (MPPLA) method. Meanwhile, the circular-shaped nanoparticles also are prepared for comparative analysis. The particle size, structure, and valence state are systematically investigated by X-ray diffraction (XRD), Raman spectra and X-ray photoelectron spectroscopy (XPS). The morphology of the nanoparticles characterized by TEM indicating the high efficient of shuttle-shaped particles in preparation. A physical model of the effect of magnetic field on the plasma plume is established to explain the formation of shuttle-shaped nanoparticles. Then, we present an explosion-absorption model to demonstrate the growth mechanism of nanoparticles. We further discuss the cluster phenomena and summarized three types of clusters in our nanoparticle suspensions. Fluorescence properties are reflected by PL spectra, which demonstrates the best performance in concentration of GaxCo0.6-xZnS0.4 with shuttle-shaped. Therefore, all the results suggest that MPPLA is promising to prepare nanoparticles since it can adjust the shape, solve the cluster and modulate performance of NPs.