This study investigated university students' perceptions of their institutions' learning environments, and related those perceptions to students' academic aspirations and satisfaction with their universities. A sample of 12,423 juniors at 42 universities in Taiwan was used to confirm the validity and reliability of the instrument: CUEI-S. The study revealed diversity of students' perceptions among specific aspects of the learning environment. Students responded more positively for student cohesion, library resources and administrative support, but less positively for student-faculty relations, student services, enhancement of their language abilities and emotional development. The majority of students had low academic aspirations but felt satisfied with their universities. The learning environment on campus was shown to play an important role both in students' academic aspirations and in their general satisfaction, whether the individual student or the university was used as the unit of analysis. The relationship between faculty and students is the aspect that was most strongly associated with students' academic aspirations. On the other hand, both adequate library resources and university support for student services were the key correlates of students' general satisfaction at the individual student level. By identifying important relationships among variables, this study suggests initiatives for improving the learning environment at higher education institutions.