A series of Co-based nanoparticles supported on activated carbon was synthesized by using waste tea leaves as a template as well as a sustainable carbon source. The crystal structure of the Co particles was adjusted by post-treatments with H 2 O 2 , ethanol vapor, and H 2 , which result in Co 3 O 4 , CoO, and metallic Co phases, respectively. After these different treatments, the composite materials consist of small Co-based nanoparticles with an average crystallite size of 6-14 nm supported on activated carbon with apparent specific surface areas up to 1065 m 2 g À 1 . Correlations between the structure of the materials and their activity for the oxygen evolution reaction (OER) were established, whereby the post-treatment with ethanol vapor was found to yield the most effective electrocatalyst. The material shows good stability at 10 mA cm À 2 over 10 h and reaches a mass activity of 2.9 A mg Co À 1 , which is even higher than pristine ordered mesoporous Co 3 O 4 . The superior electrocatalytic performance is ascribed to a high dispersion of Cobased nanoparticles and the conductivity of the activated carbon that facilitate the charge transport.