Abstract: In order to investigate the effect of preparation methods on hydrogen adsorption of bimetallic organic frameworks, CoNi-MOF-74 was prepared by direct synthesis and post-synthetic ion exchange methods, respectively. The structure and morphology of the prepared CoNi-MOF-74 were characterized by XRD, SEM, ICP and N₂ physical adsorption-desorption isotherm. In addition, hydrogen adsorption performance was further measured at 77 K and 100 kPa. The results show that the preparation method has significant effects on hydrogen adsorption. The hydrogen adsorption capacity of the CoNi-MOF-74 prepared by one-pot synthesis was up to 2.12% (m(Co): m(Ni) = 1;1), which was 24.7% higher than Ni-MOF-74 and 3.4% higher than CoNi-MOF-74 prepared by post-synthetic ion exchange. This preparation process is simple and efficient, which is beneficial for large-scale production.