The increase in cybersecurity threats and the challenges for organisations to protect their information technology assets has made adherence to organisational security control processes and procedures a critical issue that needs to be adequately addressed. Drawing insight from organisational theory literature, we develop a multi-theory model, combining the elements of the theory of planned behaviour, competing value framework, and technology—organisational and environmental theory to examine how the organisational mechanisms interact with espoused cultural values and employee cognitive belief to influence cybersecurity control procedures. Using a structured questionnaire, we deployed structural equation modelling (SEM) to analyse the survey data obtained from public sector information technology organisations in Nigeria to test the hypothesis on the relationship of socio-organisational mechanisms and techno-cultural factors with other key determinants of employee security behaviour. The results showed that knowledge of cybersecurity and employee cognitive belief significantly influence the employees’ intentions to comply with organisational cybersecurity control mechanisms. The research further noted that the influence of organisational elements such as leadership on employee security behaviour is mediated by espoused cultural values while the impact of employee cognitive belief is moderated by security technologies. For effective cybersecurity compliance, leaders and policymakers are therefore to promote organisational security initiatives that ensure incorporation of cybersecurity principles and practices into job descriptions, routines, and processes. This study contributes to behavioural security research by highlighting the critical role of leadership and cultural values in fostering organisational adherence to prescribed security control mechanisms.