In this study, we conducted a comparison between surface-observed total cloud cover (TCCs) and Moderate Resolution Imaging Spectroradiometer (MODIS)-derived total cloud cover (TCCm) over China. A statistical method was applied to estimate the average field of view (FOV) of surface observers, and the radius range of FOV was 20-25, 25-35, 35-50, and 25-45 km for spring, summer, autumn, and winter, respectively. More differences would be added in the comparison when the satellite's FOV was smaller or larger than the average FOV. Monthly mean TCCs was 74.78%, 74.41%, 66.5%, and 74.06% for each season and the corresponding TCCm was 75.27%, 78.34%, 73.82%, and 82.12%. The correlation between two data sets was stronger in spring (0.727) and summer (0.736) than in autumn (0.710) and winter (0.667). Over 60% of the differences were within the −10% to 10% range, and more differences occurred for smaller TCCs. As a special feature, we found that the dust, haze, and snow cover over specific regions in China were the possible causes of the significant differences. Generally, these two data sets were in good agreement over China, and can complement each other especially in those significant difference cases to provide more accurate TCC data sets.