Among the nondestructive carbon material characterization tools, the prominence of visible Raman spectroscopy has surged remarkably for many years due to its ability to explore a diverse array of carbon bonding configurations. However, to fully unlock the distinctive features concealed within carbon composite materials, additional specimen treatments or precise spectroscope calibrations are necessary. In the same regard, the tiny diamond grain size (5–10 nm) and the pronounced amount of sp2 carbon in the ultrananocrystalline diamond film represent major challenges in visible light excitation. In this work, we employ calibrated oxygen plasma reactive ion etching conditions to manifest the nanodiamond visible Raman signature from ultrananocrystalline diamond/amorphous carbon composite (UNCD/a‐C) films fabricated by coaxial arc plasma deposition. Upon plasma etching, the broad defect band in the visible Raman spectra converged toward the diamond characteristic Raman peak at 1332 cm−1. A detailed explanation of band components of the Raman spectra is extracted through peak fitting procedures. The results of Raman spectroscopy are further correlated with the electrical characteristics of the nitrogen‐doped UNCD/a‐C films due to the optimized oxygen plasma etching processes.