Roadmaps for India’s energy future foresee that coal power will continue to play a considerable role until the middle of the 21st century. Among other options, carbon capture and storage (CCS) is being considered as a potential technology for decarbonising the power sector. Consequently, it is important to quantify the relative benefits and trade-offs of coal-CCS in comparison to its competing renewable power sources from multiple sustainability perspectives. In this paper, we assess coal-CCS pathways in India up to 2050 and compare coal-CCS with conventional coal, solar PV and wind power sources through an integrated assessment approach coupled with a nexus perspective (energy-cost-climate-water nexus). Our levelized costs assessment reveals that coal-CCS is expensive and significant cost reductions would be needed for CCS to compete in the Indian power market. In addition, although carbon pricing could make coal-CCS competitive in relation to conventional coal power plants, it cannot influence the lack of competitiveness of coal-CCS with respect to renewables. From a climate perspective, CCS can significantly reduce the life cycle GHG emissions of conventional coal power plants, but renewables are better positioned than coal-CCS if the goal is ambitious climate change mitigation. Our water footprint assessment reveals that coal-CCS consumes an enormous volume of water resources in comparison to conventional coal and, in particular, to renewables. To conclude, our findings highlight that coal-CCS not only suffers from typical new technology development related challenges—such as a lack of technical potential assessments and necessary support infrastructure, and high costs—but also from severe resource constraints (especially water) in an era of global warming and the competition from outperforming renewable power sources. Our study, therefore, adds a considerable level of techno-economic and environmental nexus specificity to the current debate about coal-based large-scale CCS and the low carbon energy transition in emerging and developing economies in the Global South.