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A synthesis was carried out and the surface morphology of carbon nanoparticles obtained in the process of laser ablation of a carbon target was studied. The synthesis was carried out in an aqueous environment using radiation from a yttrium aluminum garnet laser (LS 2134D) with a wavelength of 1064 nm. A two pulses laser mode was used. The pulses were separated by a time interval of 3 μ s. The pulse duration was 10 ns, the pulse repetition rate was 10 Hz, and the energy of a single pulse was 0.05 J. It has been shown that during laser ablation a set of nanoparticles of various sizes and shapes is formed. The possibility of controlling the process of ablation and synthesis of carbon nanoparticles has been demonstrated. Efficient generation of nanoparticles for use in various applications has been achieved.