Leaf area index (LAI) is a terrestrial essential climate variable that is required in a variety of ecosystem and climate models. The Global LAnd Surface Satellite (GLASS) LAI product has been widely used, but its current version (V5) from Moderate Resolution Imaging Spectroradiometer (MODIS) data has several limitations, such as frequent temporal fluctuation, large data gaps, high dependence on the quality of surface reflectance, and low computational efficiency. To address these issues, this paper presents a deep learning model to generate a new version of the LAI product (V6) at 250-m resolution from MODIS data from 2000 onward. Unlike most existing algorithms that estimate one LAI value at one time for each pixel, this model estimates LAI for 2 years simultaneously. Three widely used LAI products (MODIS C6, GLASS V5, and PROBA-V V1) are used to generate global representative time-series LAI training samples using K-means clustering analysis and least difference criteria. We explore four machine learning models, the general regression neural network (GRNN), long short-term memory (LSTM), gated recurrent unit (GRU), and Bidirectional LSTM (Bi-LSTM), and identify Bi-LSTM as the best model for product generation. This new product is directly validated using 79 high-resolution LAI reference maps from three in situ observation networks. The results show that GLASS V6 LAI achieves higher accuracy, with a root mean square (RMSE) of 0.92 at 250 m and 0.86 at 500 m, while the RMSE is 0.98 for PROBA-V at 300 m, 1.08 for GLASS V5, and 0.95 for MODIS C6 both at 500 m. Spatial and temporal consistency analyses also demonstrate that the GLASS V6 LAI product is more spatiotemporally continuous and has higher quality in terms of presenting more realistic temporal LAI dynamics when the surface reflectance is absent for a long period owing to persistent cloud/aerosol contaminations. The results indicate that the new Bi-LSTM deep learning model runs significantly faster than the GLASS V5 algorithm, avoids the reconstruction of surface reflectance data, and is resistant to the noises (cloud and snow contamination) or missing values contained in surface reflectance than other methods, as the Bi-LSTM can effectively extract information across the entire time series of surface reflectance rather than a single time point. To our knowledge, this is the first global time-series LAI product at the 250-m spatial resolution that is freely available to the public (www.geodata.cn and www.glass.umd.edu).