At the 2016 Summer Olympics Schmitt won a gold medal in the 4×200 meter freestyle relay and a silver medal in the 4×100 m freestyle relay. It was the first Olympics where she served as captain of the US Olympic swim team. Schmitt was the only second-time captain for the US Olympic swim team at the 2020 Summer Olympics. At the 2020 Olympics, Schmitt won a bronze medal in the 4×100-meter freestyle relay, swimming in the prelims of the race, and a silver medal swimming in the final of the 4x200-meter freestyle relay.