The development of cheap and high-performance catalysts for the hydrolysis of ammonia borane (AB) for hydrogen production is a hotspot in the field of nanocatalysis and hydrogen energy. In this paper, we report the simple synthesis of CuO-Co 3 O 4 composite nanoplatelets that were characterized by X-ray powder diffraction, scanning electron microscopy, transmission electron microscopy, and X-ray photoelectron spectroscopy. The effects of the molar ratios of CuO to Co 3 O 4 in the composites and the calcination temperatures on the catalytic activity of the obtained products in AB hydrolysis were investigated. In addition, the active species of the catalysts and the synergy of the CuO-Co 3 O 4 nanoplatelets in AB were explored. It was determined that the turnover frequency of the CuO-Co 3 O 4 nanoplatelets can reach 33.4 min −1 . By incorporating CuO into Co 3 O 4 , the reducibility of the resultant CuO-Co 3 O 4 nanoplatelets was remarkably improved, leading to enhanced catalytic performance. The active species is the CoCu alloy formed on the surface of CuO-Co 3 O 4 by the coreduction of CuO and Co 3 O 4 with AB. These findings can help to better understand the catalytic behavior of oxide compositebased catalysts and the design of other inexpensive, high-performance catalysts.