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Clouds play a crucial role in regulating the hydrologic cycle and Earth's radiative energy budget, yet they are often poorly represented in global climate models (GCMs). This study applies deep machine learning techniques to develop a physical parameterization of volumetric cloud fraction (VCF), the fraction of a 3-D grid volume occupied by clouds using satellite lidar-radar measurements. The neural network (NN) captures the complicated relationships between observed VCF profiles and collocated meteorological variables from MERRA-2 reanalysis data. Our results show that the NN model, particularly a sequence-to-sequence long short-term memory (LSTM) network with a sixfactor loss function, effectively learns the underlying cloud physical processes. The NN model outperforms MERRA-2 reanalysis in representing low-level clouds in tropical and subtropical regions and low- and middle-level clouds over midlatitude storm-track regions, and also improves VCF histograms. These improvements are reflected in the vertical distributions of zonally, meridionally, and globally averaged VCFs, geographic distributions of low-, middle-, and high-level clouds, and seasonal variations in monthly-mean VCF. Furthermore, the NN predictions effectively capture the El Niño-Southern Oscillation (ENSO) effects and other interannual variations. The NN parameterization is further evaluated through a sensitivity analysis, in which a single predictor is perturbed at a time. This reveals that relative humidity (RH) is the dominant factor influencing variations in globally averaged VCF at low and middle altitudes, followed by temperature. At higher altitudes, temperature becomes the primary driver of VCF through its effect on RH. Changes in wind components had minimal impact on globally averaged VCF.