An ArF excimer laser (22 ns, 193 nm) and a hybrid dye/excimer laser system (500 fs, 248 nm) are used to deposit amorphous carbon nitride films at room temperature by ablation of a graphite target in nitrogen atmosphere. The chemical composition and structure of the films is characterized by X-ray photoelectron spectroscopy. In the nanosecond case, the nitrogen content increases with reactive gas pressure up to 45 atomic %, while in the subpicosecond case it remains below 7 at. %. When processed with nanosecond pulses, the films’ nitrogen content steeply increases with fluence up to a maximum. The target-to-substrate distance has only minor influence on the amount of nitrogen incorporated into the films. The dependence of the carbon–carbon and carbon–nitrogen bond configurations on the processing parameters is also given.