Cloud services have been widely regarded as a useful tool to support collaboration. However, exploring the intention to use cloud services in collaboration contexts among students who enroll in private vocational universities in Taiwan has received little scholarly attention. Most of these students are low academic achievers or not very interested in learning, which has become a great challenge to their teachers. Previous studies have indicated that collaboration among students is beneficial to their learning. Accordingly, in this study, cloud services were used to facilitate student collaboration and to further understand their intention to use such services. The results show that facilitating conditions significantly influence perceived ease of use and attitude toward using and social influence greatly affects perceived usefulness and behavioral intention. These results imply that the educational training or problem solving involved in using cloud services can help make students aware that the services are easy to use and can generate a positive attitude toward using them and that the opinions expressed by teachers or classmates are valuable with regard to leading to a belief that the services are useful for learning and contribute to behavioral intention.