Children's understanding of the concepts of teaching and learning is closely associated with their theory of mind (ToM) ability and vital for school readiness. This study aimed to develop and validate a Preschool Teaching and Learning Comprehension Index (PTLCI) across cultures and examine the causal relationship between children's comprehension of teaching and learning and their mental state understanding. Two hundred and twelve children from 3 to 6 years of age from Hong Kong and the United States participated in study. The results suggested strong construct validity of the PTLCI, and its measurement and structural equivalence within and across cultures. ToM and PTLCI were significantly correlated with a medium effect size, even after controlling for age, and language ability. Hong Kong children outperformed their American counterparts in both ToM and PTLCI. Competing structural equation models suggested that children's performance on the PTLCI causally predicted their ToM across countries.[Copyright © 2017 Wang, Wang and Chui.]