ABSTRACT Leaf nitrogen content (LNC) is an essential indicator of crop nitrogen status. To rapidly and correctly estimate the LNC using hyperspectral remote sensing, the canopy hyperspectral reflectance of coffee trees treated with five levels of nitrogen fertilization in a greenhouse was obtained in this study. Five methods were used for hyperspectral data preprocessing, namely, Savitzky–Golay (SG) smoothing, a combination of SG and standard normal variate transformation (SG-SNV), a combination of SG and first-order derivative (SG-FD), a combination of SG and second-order derivative (SG-SD), and a combination of SG and multiplicative scatter correction (SG-MSC). Feature wavelengths were extracted using variables combination population analysis (VCPA), competitive adaptive reweighted sampling (CARS), and the combination (CARS-SPA) of CARS and successive projections algorithm (SPA). Vegetation indexes (VIs) were constructed and subjected to correlation analysis and variance inflation factor (VIF) analysis. Linear and nonlinear models including partial least squares regression (PLSR), back propagation neural network (BPNN), extreme learning machine (ELM), random forest regression (RFR), and support vector regression (SVR), were adopted to construct LNC retrieval models for coffee trees. The results indicated that SG-MSC could increase the signal-to-noise ratio of hyperspectral data well. The wavelengths selected by CARS-SPA were more relevant to LNC, and combined with ELM resulted in the best performance of LNC prediction (R2 P = 0.901, RMSEP = 0.825 g·kg−1, RPD = 3.229). Ten VIs were obtained through correlation analysis and VIF, and the VIs-based ELM prediction model also performed moderately well (R2 P = 0.814, RMSEP = 1.131 g·kg−1, RPD = 2.354). By comparing the coffee LNC prediction models established by different methods, two coffee LNC inversion models with better prediction accuracy were obtained, which provide a scientific basis for accurate diagnosis of coffee trees LNC, and are of great significance for optimizing the field management.