In this study, an augmented reality-based mobile learning system is proposed for conducting inquiry-based learning activities. An experiment has been conducted to examine the effectiveness of the proposed approach in terms of learning achievements and motivations. The subjects were 57 fourth graders from two classes taught by the same teacher in an elementary school in northern Taiwan. The experimental results showed that the proposed approach is able to improve the students’ learning achievements. Moreover, it was found that the students who learned with the augmented reality-based mobile learning approach showed significantly higher motivations in the attention, confidence, and relevance dimensions than those who learned with the conventional inquiry-based mobile learning approach.