Easily processed, well-defined, and hierarchical uniform artificial architectures with intrinsic strong crystalline emission properties are necessary for a range of light-emitting optoelectronic devices. Herein, we designed and prepared ordered supramolecular spherulites, comprising planar conformational molecules as primary structures and multiple hydrogen bonds as physical cross-links. Compared with serious aggregation-induced fluorescence quenching (up to 70%), these highly ordered architectures exhibited unique and robust crystalline emission with a high PLQY of 55%, which was much higher than those of other terfluorenes. The primary reasons for the high PLQY are the uniform exciton energetic landscape created in the planar conformation and the highly ordered molecular packing in spherulite. Meanwhile, minimal residual defect (green-band) emissions are effectively suppressed in our oriented crystalline framework, whereas the strong and stable blue light radiations are promoted. These findings may confirm that supramolecular ordered artificial architectures may offer higher control and tunability for optoelectronic applications.