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The uncertainty from the under-estimation and over-estimation of forest aboveground biomass (AGB) is an urgent problem in optical remote sensing estimation. In order to more accurately estimate the AGB of <i>Pinus densata</i> forests in Shangri-La City, we mainly discuss three non-parametric models—the artificial neural network (ANN), random forests (RFs), and the quantile regression neural network (QRNN) based on 146 sample plots and Sentinel-2 images in Shangri-La City, China. Moreover, we selected the corresponding optical quartile models with the lowest mean error at each AGB segment to combine as the best QRNN (QRNNb). The results showed that: (1) for the whole biomass segment, the QRNNb has the best fitting performance compared with the ANN and RFs, the ANN has the lowest R² (0.602) and the highest RMSE (48.180 Mg/ha), and the difference between the QRNNb and RFs is not apparent. (2) For the different biomass segments, the QRNNb has a better performance. Especially when AGB is lower than 40 Mg/ha, the QRNNb has the highest R² of 0.961 and the lowest RMSE of 1.733 (Mg/ha). Meanwhile, when AGB is larger than 160 Mg/ha, the QRNNb has the highest R² of 0.867 and the lowest RMSE of 18.203 Mg/ha. This indicates that the QRNNb is more robust and can improve the over-estimation and under-estimation in AGB estimation. This means that the QRNNb combined with the optimal quantile model of each biomass segment provides a method with more potential for reducing the uncertainties in AGB estimation using optical remote sensing images.