In this study, tobermorite was successfully synthesized from two kinds of industrial wastes by single step hydrothermal method. The structural and morphological changes during synthesis show that well-crystallized tobermorite can be obtained within 6h at 180°C in this system. The carbon impurities lead to a longer synthesis time and lower crystallinity of tobermorite. The tobermorite displays attractive adsorption capacity for Cr3+ (4.87mmol/g), which is 2–3 times higher than common clay minerals. Meanwhile, Cr3+ adsorption causes the exsolution of structural Ca2+ in tobermorite channels, leading to the damage of crystallinity and decrease in sorption capacity of adsorbent. Therefore, better crystallization of tobermorite is helpful to achieve higher sorption capacity for Cr3+. These results indicate tobermorite can be used in industrial processes to adsorb heavy metals from wastewater.