The morphology of materials has a huge impact on their properties and functions; however, the precise control and direct evolution toward specific morphologies remains challenging. Herein, we outline a novel strategy for the morphology modulation of covalent organic frameworks based on COF-300 with the diamond structure, which usually exhibits a three-dimensional shuttle morphology. A monofunctional structural regulator has been designed to break the continuity of the three-dimensional structure. As the proportion of the monofunctional structural regulator increases, the morphology of COF-300 shows a directional evolution from a shuttle morphology to a two-dimensional nanosheet, while still retaining the consistency of the crystal structure. Our study reports the first two-dimensional nanosheet based on a three-dimensional structured COF to date and will inspire future research into the traced morphological evolution in materials by predesign.