Augmented Reality (AR) technology, as one of the emerging innovative technologies, is proven to have the potential to facilitate second language acquisition in terms of contextualized visualization and learning interactivity. Nevertheless, no empirical research has been conducted on the use of an AR-assisted approach to help adult Chinese language learners (CFL) acquire Chinese characters, which is a major challenge in CFL education. This study utilized a quasi-experimental research method to examine the effects of the AR-assisted approach on adult CFL learners' Chinese character recognition, writing, and memorization, as well as their attitudes and perceptions toward this kind of learning approach. Fifty elementary CFL learners, divided into an AR learning group and a traditional learning group, participated in this study. The results indicated that 1) the AR-assisted approach facilitated the recognition of semantic traits of a Chinese character, but not its morphological and phonological features, that 2) the AR-assisted approach enhanced the learners' command of the stroke order of a Chinese character but did not aid in writing the overall structure of a character, that 3) the AR-assisted approach promoted the memorization of the meaning of a character, however, failed to extend the memory retention of other aspects of the character, and that 4) learners were generally interested in the AR-assisted approach and held positive attitudes toward it, willing to use it more in their future education. In a word, the AR-assisted approach is worth trying in Chinese character acquisition for adult CFL learners though it still needs improvement.