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Adv."],"published-print":{"date-parts":[[2026,10,16]]},"abstract":"<jats:p>\n                    The interplay between coherent (wave-like) and incoherent (particle-like) phonon transport is central to heat conduction, yet experimental evidence of their crossover in bulk three-dimensional (3D) crystals remains scarce. Here, we report intrinsically ultralow lattice thermal conductivity (\n                    <jats:inline-formula>\n                      <mml:math xmlns:mml=\"http:\/\/www.w3.org\/1998\/Math\/MathML\" display=\"inline\" overflow=\"scroll\">\n                        <mml:mrow>\n                          <mml:msub>\n                            <mml:mi mathvariant=\"normal\">\u03ba<\/mml:mi>\n                            <mml:mi mathvariant=\"normal\">l<\/mml:mi>\n                          <\/mml:msub>\n                        <\/mml:mrow>\n                      <\/mml:math>\n                    <\/jats:inline-formula>\n                    ) in the lead-free double perovskite Cs\n                    <jats:sub>2<\/jats:sub>\n                    AgBiCl\n                    <jats:sub>6<\/jats:sub>\n                    , reaching 0.52 and 0.28 W\u00a0m\n                    <jats:sup>\u22121<\/jats:sup>\n                    \u00a0K\n                    <jats:sup>\u22121<\/jats:sup>\n                    in single crystal and polycrystals, respectively, at room temperature. Combining thermal transport, low-temperature heat capacity, Raman spectroscopy, synchrotron x-ray pair distribution function analysis, and anharmonic lattice-dynamics calculations, we uncover the microscopic origin of this anomalous heat transport. Chemical bonding heterogeneity, weakly bound rattling-like Cs vibrations, anisotropic Cl dynamics, and soft lattice modes generate low-energy localized optical phonons that strongly interact with acoustic modes. Enhanced three- and four-phonon scattering suppresses phonon lifetimes, while anharmonic renormalization flattens optical branches and reduces group velocities. Coherent contributions account for \u223c50% of\n                    <jats:inline-formula>\n                      <mml:math xmlns:mml=\"http:\/\/www.w3.org\/1998\/Math\/MathML\" display=\"inline\" overflow=\"scroll\">\n                        <mml:mrow>\n                          <mml:msub>\n                            <mml:mi mathvariant=\"normal\">\u03ba<\/mml:mi>\n                            <mml:mi mathvariant=\"normal\">l<\/mml:mi>\n                          <\/mml:msub>\n                        <\/mml:mrow>\n                      <\/mml:math>\n                    <\/jats:inline-formula>\n                    near room temperature and exceeding incoherent contributions above \u223c200 K, revealing an emergent coherent-incoherent phonon crossover in a fully crystalline 3D solid.\n                  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