In delivering on the world’s climate goals, removing carbon dioxide from the atmosphere is required in addition to deep mitigation efforts. As no carbon dioxide removal method stands out as an obvious winner, which, how, and how much of these technologies should be deployed to guarantee efficient, sustainable and permanent carbon dioxide removal remains a fundamental research challenge. One potential option, bioenergy with carbon capture and storage (BECCS) is likely to play an important role. BECCS’s ability to sustainably remove carbon dioxide from the atmosphere is, however, controversial. Given the range of potential outcomes, it is crucial to understand how, if at all, this technology can be deployed in a way which minimises its cost and impact on natural resources and ecosystems, while maximising both carbon removal and energy production. In this dissertation, we explore the regional drivers of BECCS sustainability and cost, and provide insights into the where, when, and extent of environmentally sustainable and economically viable BECCS deployment. We conclude that the total quantity of atmospheric carbon dioxide removal and energy production over the lifetime of a BECCS project, and the time required to start removing carbon dioxide from the atmosphere will likely vary from project to project. This has profound implications for the policy frameworks required to incentivise and regulate the widespread deployment of BECCS technology. When optimising regional biomass supply chains, we find that a myopic focus on energy generation and carbon dioxide removal can result in negative consequences for the broader environment, which warrants consideration for all impacts when assessing the performance of a BECCS project. Finally, when exploring least-cost BECCS deployment pathways to meet global carbon dioxide removal targets, an important finding is that inter-regional cooperation and collaboration are central to sustainably and affordably meeting these targets, with important value creation opportunities for key providers of carbon dioxide removal.