As the world's largest loess deposit region, the Loess Plateau's vegetation dynamics are crucial for its regional water-heat balance and ecosystem functioning. Leaf Area Index (LAI) serves as a key indicator bridging canopy architecture and plant physiological activities. Existing studies have made significant advancements in simulating LAI, yet accurate LAI simulation remains challenging. To address this challenge and gain deeper insights into the environmental controls of LAI, this study aims to accurately simulate LAI in the Loess Plateau using deep learning models and to elucidate the spatiotemporal influence of soil moisture and temperature on LAI dynamics. For this purpose, we used three deep learning models, namely Artificial Neural Network (ANN), Long Short-Term Memory (LSTM), and Interpretable Multivariable (IMV)-LSTM, to simulate LAI in the Loess Plateau, only using soil moisture and temperature as inputs. Results indicated that our approach outperformed traditional models and effectively captured LAI variations across different vegetation types. The attention analysis revealed that soil moisture mainly influenced LAI in the arid northwest and temperature was the predominant effect in the humid southeast. Seasonally, soil moisture was crucial in spring and summer, notably in grasslands and croplands, whereas temperature dominated in autumn and winter. Notably, forests had the longest temperature-sensitive periods. As LAI increased, soil moisture became more influential, and at peak LAI, both factors exerted varying controls on different vegetation types. These findings demonstrated the strength of deep learning for simulating vegetation-climate interactions and provided insights into hydrothermal regulation mechanisms in semiarid regions.