Crystalline carbon nitride nanopowders and nanorods have been successfully synthesized at room temperature and pressure using the novel technique of pulsed laser ablation of a graphite target in liquid ammonia solution. High-resolution transmission electron microscopy (HRTEM), selected area electron diffraction (SAED), and Fourier transform infrared spectroscopy (FTIR) were used to systematically study the morphology, nanostructure and chemical bonding. The experimental composition and structure of the nanoparticles are consistent with the theoretical calculations for α-C3N4. After 2 h ablation the particles had a size distribution ∼8–12 nm, whereas after 5 h ablation the particles had grown into nanorod-like structures with a crystalline C3N4 tip. A formation mechanism for these nanorods is proposed whereby nanoparticles are first synthesized via rapid formation of an embryonic particle, followed by a slow growth, eventually leading to a one-dimensional nanorod structure.