Ultrasound irradiation as an environmentally friendly and inexpensive method successfully applied for the synthesis of two-dimensional (2D) and three-dimensional (3D) metal–organic frameworks (MOFs). Sonochemically synthesized AM-Co1 and AM-Co2 powder has been employed as a green heterogeneous catalyst for the oxidative amidation reaction. The results show that AM-Co1 with a two-dimensional (2D) structure can act as an excellent catalyst for this reaction under ultrasonic irradiation compared to AM-Co2 with a three-dimensional (3D) structure. According to green principles, we used water as a green solvent and air as an oxidant for the oxidative amidation reaction. A wide variety of aldehydes and amines have been used for the synthesis of amides in good to excellent yields (75–90%). Also, the MOF catalyst could be recovered and reused several times without loss of activity.