Cold atmospheric‐pressure plasma jet not only modifies surface morphology but also introduces functional groups on sample surfaces. In this work, TiO2 nanorods/carbon fiber (TNCF) is hydrothermally prepared, and hydrogen‐doped TNCF (H:TNCF) is obtained by the surface treatment of TNCF using cold atmospheric‐pressure Ar/H2 Plasma jet. H and OH spectral lines are observed from the emitting spectrum of atmospheric‐pressure Ar/H2 plasma jet. Nanoscaled protrusions appear at top of TiO2 nanorods after the surface treatment of cold atmospheric‐pressure Ar/H2 plasma jet. OH functional groups form on the surface of H:TNCF, based on the results of FTIR, Raman and XPS analysis. Furthermore, hydrogen doping can lower the band gap from 3.2 eV of TNCF to 2.9 eV of H:TNCF, and reduce the work function from 4.97 eV of TNCF to 4.71 eV of H:TNCF. Field emission property and cell compatibility of TNCF and H:TNCF are investigated. Field emission property of TNCF is considerably improved by hydrogen doping, due to a reduced work function and a higher field enhancement factor. In the cell attachment experiments, H:TNCF exhibits more attached cells with a larger cell attachment area, compared with the TNCF sample. The obtained results show H:TNCF prepared by hydrothermal method combined with cold atmospheric‐pressure Ar/H2 Plasma jet will be a promising candidate for field emission and biocompatibility applications.