To enhance the accuracy of multispectral detection using unmanned aerial vehicles (UAVs), multispectral data of jujube fruit with different soluble solids content (SSC) and moisture content (MC) were obtained under different relative azimuth angles. Prediction models for SSC and MC of jujube fruit were established using partial least squares regression (PLSR) and support vector machines (SVM), respectively. The findings revealed that the MC of jujube fruit had the best prediction effect when the relative azimuth angle was 90°, while the SSC of the jujube fruit had the best prediction effect at an azimuth angle of 180°. Then, the spectral reflectance data corresponding to the eight relative azimuth angles were used as input variables to establish a jujube fruit quality detection model. The results showed that the prediction model for MC and SSC, established using the angle fusion method, had higher detection accuracy compared to the prediction model established at a single angle. This research provides a technical reference for improving the accuracy of outdoor jujube fruit quality detection using spectral technology.