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Cement manufacturing is one of the most energy and CO2 intensive industries. With the growth of cement production, CO2 emissions are increasing rapidly too. Carbon capture and storage is the most feasible new technology option to reduce CO2 emissions in the cement industry. More research on environmental impacts is required to provide the theoretical basis for the implementation of carbon capture and storage in cement production. In this paper, GaBi software and scenario analysis were employed to quantitatively analyze and compare the environmental impacts of cement production with and without carbon capture and storage technology, from the perspective of a life-cycle assessment; aiming to promote sustainable development of the cement industry. Results of two carbon capture and storage scenarios show decreases in the impacts of global warming potential and some environmental impacts. However, other scenarios show a significant increase in other environmental impacts. In particular, post-combustion carbon capture technology can bring a more pronounced increase in toxicity potential. Therefore, effective measures must be taken into account to reduce the impact of toxicity when carbon capture and storage is employed in cement production. CO2 transport and storage account for only a small proportion of environmental impacts. For post-combustion carbon capture, most of the environmental impacts come from the unit of combined heat and power and carbon capture, with the background production of MonoEthanolAmine contributing significantly. In combined heat and power plants, natural gas is more advantageous than a 10% coal-saving, and thermal efficiency is a key parameter affecting the environmental impacts. Future research should focus on exploring cleaner and effective absorbents or seeking the alternative fuel in combined heat and power plants for post-combustion carbon capture. If the power industry is the first to deploy carbon capture and storage, oxy-combustion carbon capture is an excellent choice for the cement industry.