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Controlled synthesis and appropriate characterization of nanoscale particles of gallium-based liquid metals are critical to fulfilling their broad range of applications in the field of flexible,stretchable,and printable micro-/nanoelectronics. Herein,we report a new way to synthesize surfactant-free gallium-indium nanoparticles with controlled particle size on a variety of substrates through a facile physical vapor deposition method.It was found that with prolonged deposition time the liquid metal nanoparticles gradually grew from near-monodispersed small particles with a diameter of~25 nm to bimodal distributed particles.A nucleation,growth,ripening and merging process was proposed to explain the observed evolution of particle size. Atomic force microscopy measurement indicates that the fabricated liquid metal nanoparticles demonstrate elastic deformation with a certain range of loads and the scanned particle size is dependent on the applied loads.We further investigated the gradual breaking process of the core-shell structured liquid metal nanoparticles, which was evidenced by multiple kinks on the force-separation curve.This work presents a new bottom-up approach to prepare nanoscale liquid metal particles and demonstrates that atomic force microscopy is a suitable technique to characterize the synthesized liquid metal nanoparticles.