Much application software education in Taiwan can hardly be regarded as practical. The researchers in this study provided a flexible means of ubiquitous learning (u-learning) with a mobile app for students to access the learning material. In addition, the authors also adopted computational thinking (CT) to help students develop practical computing skills. Three classes of first-year students were chosen for the empirical study. They were divided into three groups: two experimental groups (CT&UL group and CT group) and one control group. According to the results in this study, students who received the treatment of u-learning could have significantly better computing skills in using PowerPoint and Word than those without. However, the treatment of web-mediated CT did not result in better development of students' computing skills in this research. Finally, the researchers expect that this study provides a design and illustration of CT in a u-learning environment for schools and educators.