Leaf chlorophyll content (LCC) is an important indicator of plant nutritional status and can be a guide for plant disease diagnosis. In this study, we took apple leaves infected with mosaic disease as a research object and extracted two types of information on spectral and textural features from hyperspectral images, with a view to realizing non-destructive detection of LCC. First, the collected hyperspectral images were preprocessed and spectral reflectance was extracted in the region of interest. Subsequently, we used the successive projections algorithm (SPA) to select the optimal wavelengths (OWs) and extracted eight basic textural features using the gray-level co-occurrence matrix (GLCM). In addition, composite spectral and textural metrics, including vegetation indices (VIs), normalized difference texture indices (NDTIs), difference texture indices (DTIs), and ratio texture indices (RTIs) were calculated. Third, we applied the maximal information coefficient (MIC) algorithm to select significant VIs and basic textures, as well as the tandem method was used to fuse the spectral and textural features. Finally, we employ support vector regression (SVR), backpropagation neural network (BPNN), and K-nearest neighbors regression (KNNR) methods to explore the efficacy of single and combined feature models for estimating LCC. The results showed that the VIs model (R2 = 0.8532, RMSE = 2.1444, RPD = 2.6179) and the NDTIs model (R2 = 0.7927, RMSE = 2.7453, RPD = 2.2032) achieved the best results among the single feature models for spectra and texture, respectively. However, textural features generally exhibit inferior regression performance compared to spectral features and are unsuitable for standalone applications. Combining textural and spectral information can potentially improve the single feature models. Specifically, when combining NDTIs with VIs as input parameters, three machine learning models outperform the best single feature model. Ultimately, SVR achieves the highest performance among the LCC regression models (R2 = 0.8665, RMSE = 1.8871, RPD = 2.7454). This study reveals that combining textural and spectral information improves the quantitative detection of LCC in apple leaves infected with mosaic disease, leading to higher estimation accuracy.