methodology for quantitative measurement of nitrogen and hydrogen atomic composition of thin carbon nitride film using time-of-flight secondary-ion-mass spectrometry is demonstrated. The nitrogen and hydrogen compositions of the film are determined by the selected ion fragment intensity ratios ICN-/IC2- and IC2H-/IC2- measured in the negative-ion-mass spectrum of the film, respectively. Absolute values for hydrogen and nitrogen atomic compositions are extracted by calibration with nuclear reaction analysis and hydrogen forward scattering methods. The measured ion fragment mass intensities were also used to characterize the structure of the carbon nitride films. The results are compared with those measured from x-ray photoemission spectroscopy.