Although the Clean Air Mercury Rule (CAMR) was recently vacated by the District of Columbia Court of Appeals, efficient mercury (Hg) capture is still an important topic for the coal-fired power plant industry. Several states have Hg emission regulations that are even more stringent than CAMR guidelines. All coals contain Hg, which is released during combustion. Significant research efforts have been made to capture this toxic element before it is released to the atmosphere where it can stay suspended and travel for great distances. A variety of approaches have been examined, among which the injection of sorbent materials such as powdered activated carbon (PAC) is the current method of choice. The work presented here examined the mercury capture capability of various carbon substrates decorated with metal nanoparticles when injected as sorbents. Sorbent injections were carried out in a Hg in air mixture for laboratory-scale screening and in a real flue gas at a coal-fired power plant. It was found that palladium-decorated carbon substrates showed excellent mercury capture capabilities, with total efficiencies greater than 90% in laboratory-scale tests. In the real flue gas, the total efficiency was on the order of similar to 60%, comparable to the benchmark commercial sorbent Darco Hg-LH, a brominated PAC, although the tested adsorbents had much lower surface areas. The results of this study are presented herein. Novel mercury capture from a coal-fired flue gas was achieved using carbon substrates decorated with palladium nanoparticles.