This thesis introduces a data-driven framework bridging the gap between neurolinguistic processing observed in the human brain and the computational mechanisms of natural language processing (NLP) systems. By establishing a direct link between advanced imaging techniques and NLP processes, it conceptualizes brain information processing as a dynamic interplay of three critical components: "what," "where," and "when", offering insights into how the brain interprets language during engagement with naturalistic narratives. This study provides compelling evidence that enhancing the alignment between brain activity and NLP systems offers mutual benefits to the fields of neurolinguistics and NLP. The research showcases how these computational models can emulate the brain's natural language processing capabilities by harnessing cutting-edge neural network technologies across various modalities—language, vision, and speech. Specifically, the thesis highlights how modern pretrained language models achieve closer brain alignment during narrative comprehension. It investigates the differential processing of language across brain regions, the timing of responses (HRF delays), and the balance between syntactic and semantic information processing. Further, the exploration of how different linguistic features align with MEG brain responses over time and find that the alignment depends on the amount of past context, indicating that the brain encodes words slightly behind the current one, awaiting more future context. Furthermore, it highlights grounded language acquisition through noisy supervision and offers a biologically plausible architecture for investigating cross-situational learning, providing interpretability, generalizability, and computational efficiency in sequence-based models. Ultimately, this research contributes valuable insights into neurolinguistics, cognitive neuroscience, and NLP.