This study investigates the solution processability of hydrogen-bonded organic frameworks (HOFs) and demonstrates their potential for fabricating continuous, high-crystalline membranes. HOFs, a type of porous crystalline material, maintain their original assembly when dispersed in solvents, as confirmed by Cryo-electron microscopy (Cryo-EM) and 3D electron diffraction. The solution processability of HOFs allows for the fabrication of diverse continuous HOF membranes with high crystallinity and porosity through solution-casting on various substrates. Among these, HOF-BTB@AAO membranes exhibit high permeance for propylene (C3H6) and excellent separation performance towards C3H6 and C3H8 (SF = 14). This continuous membrane presents a green, low-cost, and efficient separation technology with potential applications in petroleum cracking and purification. The study highlights the unique solution processibility of HOFs, which enables the fabrication of continuous membranes with high crystallinity and porosity. The HOF-BTB material, constructed from the triangular building block 1,3,5-tris(4-carboxyphenyl)benzene (BTB), forms 2D honeycomb-like layers that interpenetrate into a complex 3D network, resulting in 1D undulated channels of -10 Å. The successful synthesis of crystalline HOF-BTB was confirmed using powder X-ray diffraction (PXRD), N2 sorption isotherms, and nonlocal density functional theory (NLDFT) pore size distributions. The HOF-BTB colloid solution exhibited a higher Zeta potential, indicating higher stability, and showed a broader peak width in 1H-NMR studies, suggesting a faster proton-exchange rate. The HOF-BTB@AAO membrane was fabricated using a solution-casting approach on a porous template, resulting in a highly crystalline and continuous membrane. The membrane demonstrated high permeance for C3H6 and excellent separation performance towards C3H6 and C3H8. The study also evaluated the separation performance of the HOF-BTB@AAO membrane for various gases, revealing that the main transport mechanism is Knudsen diffusion, but the membrane also exhibited a molecular sieving diffusion mechanism for gas separation, demonstrating promising potential for propane-related separation. The membrane showed robustness, high selectivity, and long-term stability for C3H6/C3H8 separation. The study provides an alternative for preparing crystalline HOF membranes with desired structure and high uniformity.This study investigates the solution processability of hydrogen-bonded organic frameworks (HOFs) and demonstrates their potential for fabricating continuous, high-crystalline membranes. HOFs, a type of porous crystalline material, maintain their original assembly when dispersed in solvents, as confirmed by Cryo-electron microscopy (Cryo-EM) and 3D electron diffraction. The solution processability of HOFs allows for the fabrication of diverse continuous HOF membranes with high crystallinity and porosity through solution-casting on various substrates. Among these, HOF-BTB@AAO membranes exhibit high permeance for propylene (C3H6) and excellent separation performance towards C3H6 and C3H8 (SF = 14). This continuous membrane presents a green, low-cost, and efficient separation technology with potential applications in petroleum cracking and purification. The study highlights the unique solution processibility of HOFs, which enables the fabrication of continuous membranes with high crystallinity and porosity. The HOF-BTB material, constructed from the triangular building block 1,3,5-tris(4-carboxyphenyl)benzene (BTB), forms 2D honeycomb-like layers that interpenetrate into a complex 3D network, resulting in 1D undulated channels of -10 Å. The successful synthesis of crystalline HOF-BTB was confirmed using powder X-ray diffraction (PXRD), N2 sorption isotherms, and nonlocal density functional theory (NLDFT) pore size distributions. The HOF-BTB colloid solution exhibited a higher Zeta potential, indicating higher stability, and showed a broader peak width in 1H-NMR studies, suggesting a faster proton-exchange rate. The HOF-BTB@AAO membrane was fabricated using a solution-casting approach on a porous template, resulting in a highly crystalline and continuous membrane. The membrane demonstrated high permeance for C3H6 and excellent separation performance towards C3H6 and C3H8. The study also evaluated the separation performance of the HOF-BTB@AAO membrane for various gases, revealing that the main transport mechanism is Knudsen diffusion, but the membrane also exhibited a molecular sieving diffusion mechanism for gas separation, demonstrating promising potential for propane-related separation. The membrane showed robustness, high selectivity, and long-term stability for C3H6/C3H8 separation. The study provides an alternative for preparing crystalline HOF membranes with desired structure and high uniformity.