Three-dimensional colloidal crystals have attracted a great deal of attention because of their potential use in photonic crystal, sensors, and other applications, but the bottlenecks in fabricating colloidal crystals include longer processing time and the lack of large-area ordered samples. A proposed capillary-enhanced method, which is a novel, efficient process for fabricating high-quality colloidal crystals in 24 h, is reported. It is necessary for increasing the processing rate by elevating the evaporation temperature but commonly resulted in the deposition of less-ordered crystals. However, high-quality colloidal crystals can be obtained in a controlled high-humidity system, resulting from the existence of secondary capillary forces present in high ambient humidity. Furthermore, the effect of secondary capillary forces will be confirmed, and it will increase with increasing humidity levels according to the semiquantitative analysis view of the surface thermodynamic behavior of small particles, including the modified Kelvin and Young-Laplace equations. Therefore, it can fine tune the relative position of the neighboring particles in the microarray and efficiently decrease the number of defects, resulting in the formation of perfect colloidal crystals with the assistance of enhanced secondary capillary forces.