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With the proposal to achieve carbon neutrality by the mid-21st century, carbon capture, utilization, and storage (CCUS) as a critical negative carbon technology is receiving extensive attention and concerns around the world. Under this context, the development of CCUS and relevant literature both have been experiencing an upsurge. However, the actual scale of CCUS is still far behind our expectations, especially, the various risks and uncertainties associated with its deployment planning have not yet been addressed clearly. Therefore, this paper provides an overview of model-based CCUS deployment pathways toward carbon neutrality, as well as the associated risks of financial, technical, environmental, health and safety (EHS) aspects. On this basis, we scrutinize the potential challenges that could lead to the pace of CCUS deployment inconsistent with the need to achieve a carbon-neutral target. The results suggest that the "Golden Age" of CCUS deployment lies from 2040 to 2060 in the world, while 2030–2050 for China. Furthermore, we found that inadequate exploration in geologic storage capacity also creates a critical conundrum for CCUS deployment and optimization, apart from typical challenges including high failure rate of projects, the lack of financial support and market stimulus, as well as incomplete regulation framework and risk-sharing mechanism. Lastly, this paper points out the further potential research direction, followed by policy implications and recommendations. • A comprehensive reference for CCUS deployment towards carbon neutrality is presented. • We discuss possible risks or uncertain factors for altering CCUS deployment paths and planning layout. • Future needs to improve geological storage exploration and estimation are highlighted. Further potential research direction and policy implications for CCUS are provided. [ABSTRACT FROM AUTHOR]