This study examined the relationship between Chinese college students' motivational needs, their attitude as well as the intention to use mobile devices for learning. The relationship between their attitude and intention of adopting mobile learning (m-learning) was also investigated. A total number of 337 Chinese college students participated in the study. Results revealed that the needs of affective, social integrative, and entertainment positively influence their attitude and intention to adopt m-learning. Additionally, entertainment needs and their attitude enhance their intention to use mobile devices for learning. This study extends the understanding of what motivates Chinese college students to adopt m-learning and also provides higher education professionals with a new vision about what influences students' attitude to use mobile devices for learning.