Due to the effect of bagging on fruit growth, non-destructive and in situ soluble solid content (SSC) in citrus detection remains a challenge. In this work, a new method for accurately quantifying SSC in citrus using hyperspectral imaging of citrus leaves was proposed. Sixty-five Ehime Kashi No. 28 citruses with surrounding leaves picked at two different times were picked for the experiment. Using the principal components analysis combined with Gaussian process regression model, the correlation coefficients of prediction-real value by citrus and its leaves in cross-validation were 0.972 and 0.986, respectively. In addition, the relationship between citrus leaves and SSC content was further explored, and the possible relationship between chlorophyll in leaves and SSC of citrus was analyzed. Comparing the quantitative analysis results by citrus and its leaves, the results show that the proposed method is a non-destructive and reliable method for determining the SSC by citrus leaves and has broad application prospects in indirect detection of citrus.