Learning content of chemistry includes factual, conceptual, procedural, and metacognitive knowledge. To well master the learning content, students' metacognition is required. Students' metacognition can be formed and developed through learning. Metacognitive learning strategy is one of the strategies that can develop and improve the metacognition of learners. The aim of this research was to develop Metacognitive Learning Strategy (MLS) to improve metacognition Chemistry Education Students' (CES). The study adopt a development research design, the 4-D model by Thiagarajan, et al. (1974). The development process consisted four steps: define, design, develop, and disseminate. Content and construct validity of MLS have been assessed by three experts. The developed MLS would be subsequently applied in the learning to increase metacognition students of CES. Improved students metacognition skills were observed using a metacognitive awareness inventory (MAI) questionnaire (Schraw & Dennison, 1994). The MLS that was developed have four steps (syntaxes), namely Preparing, Doing, Checking, and Assessing & Followingup (PDCA). Validation results indicate that PDCA's MLS is appropriate for use in learning (reliability for relevance and consistency aspects are 0.89 and 0.88 respectively). Application of MLS in organic chemistry learning was able to increase students' metacognition of CES both metacognitive knowledge and metacognitive skills with N-Gain scores () 0.31 and 0.35 respectively.