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Although it is well recognized that teaching and learning are of vital importance for the evolution of human beings, the underlying neurocognitive mechanism remains unclear. To address this issue, during the past decade we have developed a naturalistic research paradigm that combines multiple techniques such as behavioural coding, noninvasive brain imaging, and computational modeling to investigate the neurocognitive mechanism of online or offline teaching and learning. By employing this paradigm, we revealed a hierarchical neurocognitive structure of teaching in which shared neurocognitive representation and interpersonal predictive coding plays key roles. Additionally, we tested the process of knowledge transmission and construction, key factors that impacts the emergence and maintenance of teacher-student relationships, as well as naturalistic teaching outside the classroom such as parenting at home, etc. We believe that these efforts will be helpful in advancing our understanding of the neurocognitive mechanism of teaching and learning and inspire more meaning research in future.