Measurements of ocean color from Geostationary Ocean Color Imager (GOCI) with a moderate spatial resolution and a high temporal frequency demonstrate high value for a number of oceanographic applications. This study aims to propose and evaluate the calibration of GOCI as needed to achieve the level of radiometric accuracy desired for ocean color studies. Previous studies reported that the GOCI retrievals of normalized water-leaving radiances (nLw) are biased high for all visible bands due to the lack of vicarious calibration. The vicarious calibration approach described here relies on the assumed constant aerosol characteristics over the open-ocean sites to accurately estimate atmospheric radiances for the two near-infrared (NIR) bands. The vicarious calibration of visible bands is performed using in situ nLw measurements and the satellite-estimated atmospheric radiance using two NIR bands over the case-1 waters. Prior to this analysis, the in situ nLw spectra in the NIR are corrected by the spectrum optimization technique based on the NIR similarity spectrum assumption. The vicarious calibration gain factors derived for all GOCI bands (except 865nm) significantly improve agreement in retrieved remote-sensing reflectance (Rrs) relative to in situ measurements. These gain factors are independent of angular geometry and possible temporal variability. To further increase the confidence in the calibration gain factors, a large data set from shipboard measurements and AERONET-OC is used in the validation process. It is shown that the absolute percentage difference of the atmospheric correction results from the vicariously calibrated GOCI system is reduced by ~6.8%.