RNA polymerase III (Pol III) synthesizes noncoding RNAs essential for translation, RNA processing, transcription regulation, and other core cellular processes. Pol III transcription levels are coordinated with nutrient availability for cellular growth, and its dysregulation is linked to disease, such as breast cancer and leukodystrophy. Despite its importance, human Pol III regulatory mechanisms remain largely uncharacterized, in part due to limited exploration of Pol III-centered protein-protein interactions (PPIs). To address this gap, we surveyed the Pol III complex interactome by leveraging a series of Pol III-specific subunit pull-down and mass spectrometry experiments. We identified over 300 novel Pol III interactors, including Pol II-related transcription factors, nuclear import factors, and splicing factors.