Covalent organic frameworks (COFs) are an emerging class of crystalline porous materials with extended networks, connected by robust covalent bonds. Due to the high designability of structures and functions, COFs have attracted much attention in various applications. However, generation of single crystalline COF over 0.1 mm is still a challenge. To address this issue, our previous work achieved a remarkable improvement by adding ionic additives into COF growth solution. Through the study of typical 3D-COF, COF-300, we successfully generated COF crystal over 0.2 mm, and proposed the mechanism underlying the influence of ionic additives toward the size of COF crystals. However, there still exists various factors in COF crystal growth that require exploration. Especially, although COFs are commonly synthesized at elevated temperature in the past decade, the use of modulator molecules is barely discussed under this condition. Therefore, in this study, we performed crystal growth experiments at different temperatures to elucidate the temperature dependence of 3D-COF crystal growth. COF-300 is chosen as the typical iminebonded 3D-COF, and aniline is used as modulator. As a result, we found that higher temperature resulted in both less nucleation and smaller sizes of COF crystals, which could be attributed to the influence of temperature on the solubility of materials. The results of this study allowed us to identify the conditions that favored the generation of larger COF crystals, contributing to the development of effective strategy toward imine-bonded 3D-COFs growth.