A crown ether-assisted supramolecular assembly method was used to create blue and green emitting halide perovskite materials with near-unity photoluminescence quantum yield (PLQY). The study demonstrated that the supramolecular assembly of Hf and Zr halide octahedral clusters, specifically (18C6@K)₂HfBr₆ and (18C6@K)₂ZrCl₄Br₂, produced blue and green emissions with high PLQY (96.2% and 82.7%, respectively). These materials were synthesized using a low-temperature solution-based method, enabling their use in solution-processable inks for thin-film displays and 3D printing. The supramolecular assembly allowed for the isolation of octahedral units, which enhanced their optoelectronic properties by reducing nonradiative recombination and increasing the efficiency of light emission. The materials exhibited strong electron-phonon coupling, leading to self-trapped exciton (STE) states and long PL lifetimes. The blue and green emissions were also stable under ambient conditions and showed high photostability. The supramolecular approach enabled the creation of dual-color displays and complex 3D architectures with high spatial resolution. The study highlights the potential of supramolecular assembly for developing efficient, solution-processable light-emitting materials with applications in optoelectronics and display technologies.A crown ether-assisted supramolecular assembly method was used to create blue and green emitting halide perovskite materials with near-unity photoluminescence quantum yield (PLQY). The study demonstrated that the supramolecular assembly of Hf and Zr halide octahedral clusters, specifically (18C6@K)₂HfBr₆ and (18C6@K)₂ZrCl₄Br₂, produced blue and green emissions with high PLQY (96.2% and 82.7%, respectively). These materials were synthesized using a low-temperature solution-based method, enabling their use in solution-processable inks for thin-film displays and 3D printing. The supramolecular assembly allowed for the isolation of octahedral units, which enhanced their optoelectronic properties by reducing nonradiative recombination and increasing the efficiency of light emission. The materials exhibited strong electron-phonon coupling, leading to self-trapped exciton (STE) states and long PL lifetimes. The blue and green emissions were also stable under ambient conditions and showed high photostability. The supramolecular approach enabled the creation of dual-color displays and complex 3D architectures with high spatial resolution. The study highlights the potential of supramolecular assembly for developing efficient, solution-processable light-emitting materials with applications in optoelectronics and display technologies.