Many scholars have focused on the advantages and characteristics of Orff Schulwerk in improving students’ music learning performance; however, the effects of students’ perceptions of Orff Schulwerk on their learning performance remain unexplored. Based on the technology acceptance model (TAM), this study explored the differences among college students of different grades in terms of Orff Schulwerk perception, music learning interests, and learning performance; the effects of students’ perceptions of Orff Schulwerk on their music learning performances and the mediating effect of music learning interest, with 433 Chinese college students majoring in preschool education as the samples. The results showed that college students of different grades show no significant differences in Orff Schulwerk perception, music learning interests, and learning performance; college students’ perceptions of Orff Schulwerk had a significant positive effect on their music learning performances, and their music learning interest had a partial mediating effect. Supplementing the theoretical literature on Orff Schulwerk, this study fills the gap in literature, extends the application of the TAM to the field of education, and provides a practical reference for colleges and universities to use Orff Schulwerk for provoking college students’ learning interest and improving their performances.