Reducing CO2 emissions is a key task of modern society to attenuate climate change and its environmental effects. Accelerated weathering of limestone (AWL) has been proposed as a tool to capture CO2 from effluent gas streams and store it primarily as bicarbonate in the marine environment. We evaluated the performance of the biggest AWL-reactor to date that was installed at a coal-fired power plant in Germany. Depending on the gas flow rate, approximately 55% of the CO2 could be removed from the flue gas. The generated product water was characterized by an up to 5-fold increase in alkalinity, which indicates the successful weathering of limestone and the long-term storage of the captured CO2. A rise of potentially harmful substances in the product water (NO2-, NOx-, NH4+, SO42-, and heavy metals) or in unreacted limestone particles (heavy metals) to levels of environmental concern could not be observed, most likely as a result of a desulfurization of the flue gas before it entered the AWL reactor. At locations where limestone and water availability is high, AWL could be used for a safe and long-term storage of CO2.