Carbon-encapsulated molybdenum nanoparticles were synthesized by laser-assisted photolysis of gaseous precursors. In the proposed method, gas mixtures containing various hydrocarbons and molybdenum hexacarbonyl vapor diluted in argon were irradiated with a nanosecond pulsed UV laser at room temperature. Particle samples were analyzed by transmission electron microscopy (TEM), electron microdiffraction (EMD), energy-dispersive X-ray spectroscopy (EDS), and high-angle annular dark-field scanning transmission electron microscopy (HAADF-STEM) techniques to observe the morphology and composition of the Mo/C nanoparticles. The influence of the type of hydrocarbon, its mole fraction, and the number of UV laser pulses on the resulting nanoparticles was investigated. The nanoparticles were heavily aggregated and consisted of Mo-based cores surrounded by carbon. The type of hydrocarbon did not have any visible effects on the nanoparticle structure and the size of the Mo-based cores or aggregates. Increasing the hydrocarbon mole fraction in the precursor mixture led to an increase in the carbon content and decrease of the Mo-based core size. Increasing the number of UV laser pulses led to larger Mo cores.