A series of carbon-doped ZnO [Zn1−yCyO (0.00 ≤ y ≤ 0.10)] nanorods were synthesized using a cost-effective low-temperature (85 °C) dip coating technique. X-ray diffractometer scans of the samples revealed the hexagonal structure of the C-doped ZnO samples, except for y = 0.10. XRD analysis confirmed a decrease in the unit cell volume after doping C into the ZnO matrix, likely due to the incorporation of carbon at oxygen sites (CO defects) resulting from ionic size differences. The morphological analysis confirmed the presence of hexagonal-shaped nanorods. X-ray photoelectron spectroscopy identified C–Zn–C bonding, i.e., CO defects, Zn–O–C bond formation, O–C–O bonding, oxygen vacancies, and sp2-bonded carbon in the C-doped ZnO structure with different compositions. We analyzed the deconvoluted PL visible broadband emission through fitted Gaussian peaks to estimate various defects for electron transition within the bandgap. Raman spectroscopy confirmed the vibrational modes of each constituent. We observed a stronger room-temperature ferromagnetic nature in the y = 0.02 composition with a magnetization of 0.0018 emu/cc, corresponding to the highest CO defects concentration and the lowest measured bandgap (3.00 eV) compared to other samples. Partial density of states analysis demonstrated that magnetism from carbon is dominant due to its p-orbitals. We anticipate that if carbon substitutes oxygen sites in the ZnO structure, the C-2p orbitals become localized and create two holes at each site, leading to enhanced p–p type interactions and strong spin interactions between carbon atoms and carriers. This phenomenon can stabilize the long-range order of room-temperature ferromagnetism properties for spintronic applications.