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This study uses augmented reality (AR) technology to implement an AR-learning system for English vocabulary learning. Although previous studies have indicated that multimedia courseware enhances learning effectiveness, some important issues may cause negative effects. This study investigates learners' satisfaction and behavioral intention as well as the effectiveness of the AR-learning system. The results of this study showed that system quality was a critical factor affecting perceived satisfaction, perceived usefulness, and AR-learning effectiveness. Perceived self-efficacy also affected perceived satisfaction and perceived usefulness. On the other hand, multimedia instruction was a minor factor affecting perceived usefulness and AR-learning effectiveness. We verified that learners' behavioral intention was affected by perceived satisfaction and perceived usefulness of the AR-learning system. Furthermore, the design of system function and operation process must be more straightforward for learners when adopting new technology in the learning system.