Naturalistic stimuli, such as movies, more closely recapitulate "real life" sensory processing and behavioral demands relative to paradigms that rely on highly distilled and repetitive stimulus presentations. The rich complexity inherent in naturalistic stimuli demands an imaging system capable of measuring spatially distributed brain responses, and analysis tools optimized for unmixing responses to concurrently presented features. In this work, the combination of passive movie viewing with high-density diffuse optical tomography (HD-DOT) is developed as a platform for naturalistic brain mapping. We imaged healthy young adults during free viewing of a feature film using HD-DOT and observed reproducible, synchronized cortical responses across a majority of the field-of-view, most prominently in hierarchical cortical areas related to visual and auditory processing, both within and between individuals. In order to more precisely interpret broad patterns of cortical synchronization, we extracted visual and auditory features from the movie stimulus and mapped the cortical responses to the features. The results demonstrate the sensitivity of HD-DOT to evoked responses during naturalistic viewing, and that feature-based decomposition strategies enable functional mapping of naturalistic stimulus processing, including human-generated speech.