As an ideal medium for the development of 21st-century skills, Computational Thinking is commonly developed through Computer Science practices such as programming and robotics. Among the vast literature on Computational Thinking, few of them address the strategy to implement Design Thinking to facilitate the development of Computational Thinking. This study investigates whether Design Thinking can facilitate the development of Computational Thinking based on a systematic literature review as a method of this research. The author identifies the literature that can be used as a reference in this study, analyzes the development of Computational Thinking skill, and looks for its correlation with Design Thinking—both Design Thinking and Computational Thinking to support problem-solving skills through a structured thinking approach.