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In particular, chiral HMHs could be endowed with fascinating chiroptoelectronic properties such as circularly polarized light emission, circularly polarized photodetection, and spin regulation. However, the implementation of their practical integrated optoelectronic applications has been mainly restricted to planar thin\u2010film devices due to the poor processability of chiral HMHs for the construction of complex three\u2010dimensional (3D) architectures. Here, we take advantage of the glass transition of chiral HMH with 3D printing technology to construct self\u2010supported 3D architectures with high\u2010performance linear and nonlinear optical functionalities. Chiral HMH (\n                    <jats:italic>R<\/jats:italic>\n                    \/\n                    <jats:italic>S<\/jats:italic>\n                    \u2010THNA)\n                    <jats:sub>3<\/jats:sub>\n                    SbCl\n                    <jats:sub>6<\/jats:sub>\n                    \u00b70.5H\n                    <jats:sub>2<\/jats:sub>\n                    O (\n                    <jats:italic>R<\/jats:italic>\n                    \/\n                    <jats:italic>S<\/jats:italic>\n                    \u2010THNA =\n                    <jats:italic>R<\/jats:italic>\n                    \/\n                    <jats:italic>S<\/jats:italic>\n                    \u20101,2,3,4\u2010tetrahydro\u20101\u2010naphthylammonium) forms transparent amorphous glass upon rapid quenching from its molten state. The resulting\n                    <jats:italic>R<\/jats:italic>\n                    \/\n                    <jats:italic>S<\/jats:italic>\n                    \u2010SbCl\u2010glass favors tunable photoluminescence colors and a large, continuously tunable range of glass transition temperature (\u223c50\u00b0C) through metal halide infusion. The intrinsic thermoplasticity of HMH glasses allows for additive\u2010free, thermally assisted extrusion\u2010based printing of self\u2010supporting 3D architectures. Upon recrystallization, the printed structures recovered non\u2010centrosymmetric crystal lattices and exhibited strong isotropic second harmonic generation response, enabling customized nonlinear optical imaging. This work establishes a thermally programmable paradigm for transforming HMHs from molecularly designed materials into 3D optical architectures.\n                  <\/jats:p>","DOI":"10.1002\/adma.75314","type":"journal-article","created":{"date-parts":[[2026,10,7]],"date-time":"2026-10-07T07:08:33Z","timestamp":1791356913000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Glass Transition of Chiral Hybrid Metal Halides for Self\u2010Supported 3D Printing"],"prefix":"10.1002","author":[{"given":"Junjie","family":"Guan","sequence":"first","affiliation":[{"name":"School of Materials Science and Engineering Tianjin Key Laboratory of Metal and Molecular Materials Chemistry Frontiers Science Center for New Organic Matter Academy for Advanced Interdisciplinary Studies National Key Laboratory of Semiconductor Laser Nankai University  Tianjin People's Republic of 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