Australia has committed to meeting its international obligations to decrease its greenhouse gas emissions including transitioning toward decarbonising its emission-intense energy sector. However, it is facing the dual problems of increasing electricity cost and decreasing energy security. One of the potential contributions to reducing its emission while supplying reliable power is deployment of bioenergy with carbon capture and storage (BECCS). BECCS is a carbon removal technology that offers permanent net removal of carbon dioxide from the atmosphere together with the prospect of negative emissions. The present study was undertaken to assess the potential contribution of BECCS to achieving long term decarbonising of the Australian energy sector. This study considers the availability of sustainable bioenergy resources and the economic viability and environmental impacts of BECCS. In order to avoid the ecological uncertainties and social challenges of dedicated energy crops, this study focuses on organic waste from the municipal, agricultural, and forestry sectors. Based on the quantity of biomass resources available, BECCS options in Australia have the potential to remove a total of 25 million tonne CO2/year from the atmosphere as negative emissions by 2050. In addition, BECCS systems could supply Australia with up to 13.7 terawatt-hours of renewable power by mid-century which is around 3.6% of expected gross electricity generation in 2050. Deployment of BECCS as a reliable supplier of electricity would potentially enhance the flexibility and diversity of Australia's energy portfolio and remove carbon dioxide from the atmosphere. However, deployment of BECCS as a carbon negative strategy will require strong policy support.