Accurate dietary intake estimation is critical for informing policies and programs to support healthy eating, as malnutrition has been directly linked to decreased quality of life. However self-reporting methods such as food diaries suffer from substantial bias. Other conventional dietary assessment techniques and emerging alternative approaches such as mobile applications incur high time costs and may necessitate trained personnel. Recent work has focused on using computer vision and machine learning to automatically estimate dietary intake from food images, but the lack of comprehensive datasets with diverse viewpoints, modalities and food annotations hinders the accuracy and realism of such methods. To address this limitation, we introduce NutritionVerse-Synth, the first large-scale dataset of 84,984 photorealistic synthetic 2D food images with associated dietary information and multimodal annotations (including depth images, instance masks, and semantic masks). Additionally, we collect a real image dataset, NutritionVerse-Real, containing 889 images of 251 dishes to evaluate realism. Leveraging these novel datasets, we develop and benchmark NutritionVerse, an empirical study of various dietary intake estimation approaches, including indirect segmentation-based and direct prediction networks. We further fine-tune models pretrained on synthetic data with real images to provide insights into the fusion of synthetic and real data. Finally, we release both datasets (NutritionVerse-Synth, NutritionVerse-Real) and the collection of models (NutritionVerse) on https://bit.ly/genai4good as part of an open initiative to accelerate machine learning for dietary sensing.