An interesting reversible shape and structure transformation between two types of two-dimensional (2D) metal-organic frameworks (MOFs) has been successfully achieved by the spray method. The ability to precisely control the morphology and structure of 2D MOFs is also developed by altering the amount of MOF precursors and reversing the spray order. Meanwhile, the mechanism of the transformation between two MOFs is studied and conversion is induced by the change of the acidity in the reaction system. In addition, the prepared non-interpenetrate CuBDC twists exhibit more remarkable catalytic performance in C-S coupling reaction than Cu(BDC)(DMF) nanosheets owing to the more unsaturated coordination copper active sites from the non-interpenetrate structure. The catalytic result reveals the relationship between structure and function.