This research is set in the field of library and information science. It aimed to explore the nature of the collaborative relationship between academics and library staff in universities through the theoretical lenses of structuration theory (Giddens, 1984) and duality of technology theory (Orlikowski, 1992a). The main research objectives were: - To identify characteristics of collaborative relationships between academics and library staff, and to differentiate between more and less effective forms of collaboration in different situations and contexts; - To elucidate the factors that constrain and enable collaboration between academics and library staff, including the role of socio-cultural factors, professional boundaries, and information technology; - To develop a theoretical framework of collaboration between academics and librarians. The scope of this research is limited to collaboration between academics and library staff in areas of teaching, learning, student academic and research skills development, and library research projects. It does not include data on the areas of research support related services such as bibliometrics, data management, publishing or research infrastructure. The research used a multiple embedded case study design to study collaboration between academics and library staff in two universities: one in Australia, and one in Vietnam. Collaboration at the Australian university was more structured and reached a wider scope of practice than its Vietnamese counterpart, but both universities’ governance systems lacked an institution-wide focus, development strategies and action plans for collaboration. There was little in the way of intersecting structures, shared missions or tasks that required library staff and academics to work together. The universities provided an imbalanced resourcing structure to support the implementation of collaboration frameworks and policies. Strategies for developing collaboration were insufficient, since libraries focused on collaboration in teaching rather than research, while faculties displayed a more research-focused orientation. Moreover, academics and library staff both faced challenges in terms of multiple roles, particularly in the case of the academics. Levels of collaboration therefore varied according to academics, faculties, libraries and campuses, but success was mainly based on relationships between participants. Both universities faced similar challenges in terms of government funding reduction, resource constraints, imbalanced collaboration structures, issues of power asymmetries, insufficient understanding of librarians’ roles, and technological issues. The situation at the Vietnamese university was harder due to its higher bureaucratic and rigid organisational structure, lower levels of development of infrastructure and facilities, limited budget, low income, and a larger social divide between academics and library staff. Differences in work culture between academics and librarians could create frustration. Academic culture emphasised a more independent working style and individualistic focus whilst library culture was more collaborative and responsive, but also more structured and detail-focused, emphasising the value of collective decisions and teamwork. In comparison with the Australian university, the work culture of both academics and library staff in the Vietnamese university was more strongly influenced by leaders’ work culture. The leaders could create either an individualistic or a collaborative environment. Different management styles presented by the university leaders (either the Western or Asian work culture) shaped the work practice of their subordinates. Findings of the similarities and differences of the two universities are important for understanding collaboration patterns that exist across the social, cultural and educational contexts and how factors in particular contexts produce different forms of collaboration. The cross-country comparisons of factors that influenced collaboration enhance understanding of how and why collaboration between academics and library staff varies from one country to another. The research findings contribute insights into the challenges of collaboration from the perspectives of library staff, academics and other involved partners, rather than solely from the library practitioners’ viewpoint. There are also national implications from this comparative study. It explicates important characteristics of the collaborative relationship in a particular country’s context including the similarities and differences in social, cultural, professional, technological structures that influence collaboration. Theoretically, the research has examined the utility of structuration theory and duality of technology theory in studying contextual factors that influence the outcomes of the academic and librarian relationship. From a social perspective, the theoretical lens of the recurring interplay between structures and practice enabled the researcher to grasp the dynamic changes in social practices, and the complex nature of a collaborative relationship, particularly different collaboration patterns that are mediated by the interplay of social power relationships, financial resources, distinctive cultural values, and norms. From an organisational perspective, structuration theory helped to explain how organisational structure enabled and constrained practices, as well as how practices influenced and transformed the structure. From a structural perspective, Giddens’ theory underlined the importance of time and space as elements of social systems that exist in instantiations of social practices. These concepts held significant implications in the findings of the presence of time and space in collaborative practice and how time and space linked with the varying levels of collaboration. From a cultural perspective, Giddens’ conceptualisation of cultural values as shared meaning systems in relation to power, norms and knowledgeability of participants led to a deeper understanding of the socio-cultural dynamics and professional culture and norms of academics and library staff. The research contributes to the literature of organizational collaboration an emergent theoretical framework of influencing factors on the collaborative relationship between academics and library staff. From a practical perspective, it offers contextual recommendations for the Australian university and the Vietnamese university, and extrapolates key insights for interested universities and practitioners in addressing the problems of collaboration in different cultural and educational contexts.