Georgios Simiriotis played all three events at the 1906 Athina Olympics, winning a silver medal in mixed doubles alongside Sofia Marinou. Simiriotis played doubles alongside Nikolaos Zarifis, losing in the semi-finals and then losing the bronze medal match to finish fourth. In singles Simiriotis lost in the quarter-finals to Dutch player Gerard Scheurleer. His sister, Esme Simiriotis, was the 1906 women’s singles gold medalist. Their mother was a descendent of the wealthy Greek banking family of Georgios Zarifis, so Georgios Simiriotis was also likely related to his doubles partner at the 1906 Olympics.