Using high-resolution imaging at negative spherical aberration of the objective lens in an aberration-corrected transmission electron microscope, we measure the concentration of oxygen in Sigma3[111] twin boundaries in BaTiO3 thin films at atomic resolution. On average, 68% of the boundary oxygen sites are occupied, and the others are left vacant. The modified Ti2O9 group unit thus formed reduces the grain boundary energy and provides a way of accommodating oxygen vacancies occurring in oxygen-deficient material by the formation of a nanotwin lamellae structure. The atomically resolved measurement technique offers the potential for studies on oxide materials in which the electronic properties sensitively depend on the local oxygen content.