The societal disturbance created by the rapid outbreak of the COVID-19 pandemic has shaken the entire globe, profoundly affecting all levels of education. The challenge presented by COVID-19 is broad, rapidly evolving, and complex; it threatens everyone’s well-being, the global economy, the environment, and all societal and cultural standards and our daily activities. Throughout the Coronavirus outbreak and any future lockdowns, it is crucial that the needs of students be ultimately and regularly met and that they are supported effectively. We intend to address skill shortages and mismatches, particularly regarding the readiness to teach in an online environment that encourages flexible and innovative learning. The main contribution of this paper is addressing this subject with an integrated vision of three different players in higher education: students, teachers and librarians. Using the Technology Adoption Model (TAM) and the Unified Theory of Acceptance and Use of Technology (UTAUT), a conceptual model was developed to explain both the behavior and intentions of users when using e-learning systems. Among Portuguese students, 91% of e-learning satisfaction can be attributed to perceived usefulness, actual use, and personal considerations. For educators, satisfaction appears to be mostly dependent on perceived usefulness and usability, while librarians’ satisfaction is negatively dependent on technological factors. Students’ actual use of technology is 89% dependent on organizational and technological variables. However, the actual use by teachers appears to be primarily dependent on personal and technological factors. Similarly, 91% of the variability of the use of e-learning tools by librarians can be explained by organizational, personal and technological factors, with the personal factors having a negative impact on the actual use.