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As a typical chemical hydride, ammonia borane (AB) has received extensive attention because of its safety and high hydrogen storage capacity. The aim of this work was to develop a cost-efficient and highly reactive catalyst for hydrolyzing AB. Herein, we synthesized a series of Cu<i>_x</i>Co_{1&#8722;<i>x</i>}MoO₄ dispersed on graphitic carbon nitride (g-C₃N₄) to dehydrogenate AB. Among those Cu<i>_x</i>Co_{1&#8722;<i>x</i>}MoO₄/g-C₃N₄ catalysts, Cu_0.4Co_0.6MoO₄/g-C₃N₄ exhibited the highest site time yield (STY) value of 75.7 <inline-formula> <math display="inline"> <semantics> <mrow> <mi mathvariant="normal">m</mi> <mi mathvariant="normal">o</mi> <msub> <mi mathvariant="normal">l</mi> <mrow> <msub> <mi mathvariant="normal">H</mi> <mn>2</mn> </msub> </mrow> </msub> <mi mathvariant="normal">m</mi> <mi mathvariant="normal">o</mi> <msub> <mi mathvariant="normal">l</mi> <mrow> <mi mathvariant="normal">c</mi> <mi mathvariant="normal">a</mi> <mi mathvariant="normal">t</mi> </mrow> </msub> <msup> <mrow></mrow> <mrow> <mo>&#8722;</mo> <mn>1</mn> </mrow> </msup> <mtext>&#8201;</mtext> <mi mathvariant="normal">m</mi> <mi mathvariant="normal">i</mi> <msup> <mi mathvariant="normal">n</mi> <mrow> <mo>&#8722;</mo> <mn>1</mn> </mrow> </msup> </mrow> </semantics> </math> </inline-formula> with a low activation energy of 14.46 kJ mol^&#8722;1. The STY value for Cu_0.4Co_0.6MoO₄/g-C₃N₄ was about 4.3 times as high as that for the unsupported Cu_0.4Co_0.6MoO₄, indicating that the g-C₃N₄ support plays a crucial role in improving the catalytic activity. Considering its low cost and high catalytic activity, our Cu_0.4Co_0.6MoO₄/g-C₃N₄ catalyst is a strong candidate for AB hydrolysis for hydrogen production in practical applications.