This research aimed to develop handout teaching materials based on the competence of 21stcentury students using Think Pair Share (TPS) learning model, find out the appropriateness of the handout, find out the students' and teachers' responses. This research and development used 4D development models including: (1) Define, (2) Design, (3) Develop, and (4) Disseminate. The instruments and data collection used were teacher interviews, questionnaire sheets of validation assessment, teachers' responses, and students' responses. The testing done in this research was limited product testing on the fourth grade of SD Negeri Kembaran. The results of this research and development of handout teaching materials fulfilled the criteria with a score of 4.34 from the validator expert which meant it was appropriate to be tested. The results stated that the teachers' response toward the assessment of handout teaching materials had an average score of 4.75 with the criteria of very good, so it could be concluded that the handout teaching materials were appropriate to be used. The assessment results of students' responses toward the handout teaching materials had average score of 4.51 which was categorized as very good. The conclusion was that the handout teaching materials could be accepted by students as teaching materials that can help their learning process.