Rapid and accurate leaf area index (LAI) determination is important to monitoring daylily growth, yield estimation, and field management. Because of low estimation accuracy of empirical models based on single-source data, we proposed a machine-learning algorithm combining optical and microwave remote-sensing data, and the random forest regression (RFR) importance score to select features. A high-precision LAI estimation model for daylilies was constructed by optimizing feature combinations. The RFR importance score screened the top five important features, including vegetation indices land surface water index (LSWI), generalized difference vegetation index (GDVI), normalized difference yellowness index (NDYI) and backscatter coefficients VV and VH. Vegetation index features characterized canopy moisture and color of daylilies, and the backscatter coefficient reflected dielectric properties and geometric structure. Selected features were sensitive to daylily LAI. The RFR algorithm had good anti-noise performance and strong fitting ability; thus, its accuracy was better than the partial least squares regression and artificial neural network models. Synergistic optical and microwave data more comprehensively reflected the physical and chemical properties of daylilies, making the RFR-VI-BC05 model after feature selection better than the others. This study expanded methods for estimating daylily LAI by combining optical and radar data, providing technical support for daylily management.