This study explores Chinese learners’ metacognition in EFL pronunciation learning as well as the effectiveness of helping the learners to improve their English pronunciation by metacognitive instructions. By means of preliminary interviews and a questionnaire survey carried out in seven universities across mainland China, six factors of metacognition in EFL pronunciation were extracted via factor analysis. These were Task Knowledge of Pronunciation Learning; Person Knowledge of Pronunciation Learning; Positive Experiences in Pronunciation Learning; Motivating Experiences in Pronunciation Learning; Learning Pronunciation by External Assistance; and Learning Pronunciation by Self-Effort. Based on Flavell’s model of metacognition, the metacognitive model of pronunciation learning was constructed. In addition, following an eight-week metacognitive instruction with weekly journals kept by the participants, dynamic changes in metacognition were discovered. Moreover, as the results of pronunciation tests before and after the instruction showed, the participants manifested increased pronunciation proficiency after the instruction, suggesting that metacognitive instructions may be effective in improving learners’ pronunciation in a foreign language. Limitations of the study are discussed, and suggestions for further research are made.