We demonstrate that a moderate plasma treatment increases the quality of optically detected magnetic resonance (ODMR) signals from negatively charged nitrogen-vacancy centres in nanodiamonds (NDs). We measured the statistics of the ODMR spectra of 50-nm-size NDs before and after plasma treatment. We then evaluated each ODMR spectrum in terms of fluorescence and ODMR intensities, line width and signal-to-noise (SN) ratio. Our results showed that plasma treatment for more than 10 min contributes to higher-quality ODMR signals, i.e. signals that are brighter, stronger, sharper and have a higher SN ratio. We showed that such signal improvement is due to alteration of the surface chemical states of the NDs by the plasma treatment. Our study contributes to the advancement of biosensing applications using ODMR of NDs.