LAUSR

Highly spatial and angular precision in epitaxial‐growth process is crucial for constructing organic low‐dimensional heterostructures (OLDHs) with the desired substructures, which remains significant challenge owing to the unpredicted location of complex heterogeneous nucleation. Herein, a dynamic epitaxial‐growth approach is developed along the tailored longitudinal/horizontal directions to create diverse OLDHs with hierarchical architectures. The controlled morphology evolution of seed crystals from kinetic to thermodynamic species is achieved via incrementally increasing the crystallization time from 0 to 600 s. Accordingly, the kinetic and thermodynamic seed crystals respectively present the specific lattice‐matching crystal‐planes of (100) and (011), which facilitates the longitudinal epitaxial‐growth (LG) process for triblock heterostructures, and the horizontal epitaxial‐growth (HG) process for axial‐branch heterostructures. The dominant core/shell heterostructures are prepared via both LG and HG processes with a crystallization time of ≈30 s. Significantly, these prepared OLDHs realize the rationally polarized exciton conversion for optical logic gate application through the exciton conversion and photon propagation at the heterojunction. This strategy provides an avenue for the precise synthesis of OLDHs with anisotropy optical characters for integrated optoelectronics.