A facile and efficient technique for synthesizing rapid and large-scale colloidal monolayer is introduced to obtain surface anisotropic particles. Silica particles grafted with long alkyl chains are rapidly organized into monolayer assemblies by implementing water-film climbing and convective particle assembly on glass slides. Assembled particles are modified into surface-anisotropic particles utilizing physical vapor deposition with a magnetically active material. The magnetic hemisphere enables separation of modified and unmodified surface-anisotropic particles. The proposed methodology can lead to a large-scale production opportunity for surface-anisotropic particles.