A facile and efficient approach is developed for the fabrication of asymmetric non-spherical polymer particle arrays. A specific amount of solvent is provided to interact with the spherical polymer particles to intensify the segmental mobility, thus suppressing the viscosity and the glass transition temperature of the polymer particles. The spherical polymer particlesin therubbery state are deformed into non-spherical particle arrays at the gas/liquid interface. The upper parts of the polymer particles that protrude out of the liquid phase undergo deformation by interfacial tensions at the three-phase contact line, allowing the formation of a ridge of polymer with a protrusion on the top surface. Simultaneously, the lower parts of the polymer particles submerged under the liquid phase are subjected to enormous surface tension at the contact points, leading to a non-linear coalescence behavior of the neighboring polymer particles.