Contaminated waste such as heavy metal and radioactive waste pose a severe threat to the environment and human health. Cement-based stabilization/solidification (S/S) methods are time- and cost-effective. However, high carbon footprint and low compatibility are major limitations of the conventional S/S method. It is important to develop a green and sustainable remediation strategy that utilizes agricultural/industrial by-products and low-carbon cement for S/S of contaminated waste. This approach can attenuate the environmental impacts as well as recycle wastes into valuable resources. This chapter introduces the applications of S/S mechanisms for specific heavy metal and radioactive waste by using low-carbon cement-based materials. It also recommends suitable cementitious materials for the S/S of specified contaminants in a sustainable manner.