Stimuli-responsive color changes have attracted much interest for development of a variety of sensors. [1-3] How to induce the color changes in response to external stimuli, such as heat, light, and force, is a key to design the molecules and materials. [4,5] For example, thermoresponsiveness is achieved by temperature-dependent gradual structure changes including chromophore. Thermochromism requires reversibility of the structure changes. However, in general, it is not easy to induce these dynamic structure changes at lower temperature, such as cryogenic range, because molecular motion becomes suppressed. Therefore, low-temperature thermoresponsive and reversible color changes are challenging targets and interesting phenomena for chemists. Visualization and quantification of cryogenic temperature range are significant for process controls in biological, medical, and food sciences and industries. Previous works showed a couple of the approaches (Figure S1, Emergence of thermoresponsive and reversible color changes at low temperature is a challenging target. In general, it is not easy to induce sufficient dynamic motion of rigid molecules including chromophore at a lower temperature. The present work shows unusually low-temperature color-change properties originating from the dynamic motion of rigid conjugated polymer in solid state. The layered composites of polydiacetylene (PDA) and guest l-arginine (L-Arg) (PDA-(L-Arg)) exhibit temperatureresponsive gradual color changes with reversibility in the range of 123-333 K in solid crystalline state. The dynamic properties are induced by gradual and reversible distortion of the π-conjugated main chain in response to temperature. The tuned flexibility of the layered structure facilitates motion of the rigid π-conjugated molecule at low temperature. The PDA-(L-Arg)-coated substrates are applied to visualization and quantification of 2D and 3D temperature distributions generated by cooling with liquid nitrogen. These thermographic devices afford to image lower temperature range than typical infrared thermography. The present work indicates potentials of layered architectures with tunable flexibility for emergence of dynamic properties. Supporting Information). [6-14] Metalorganic frameworks consisting of lanthanide ions and photo-responsive ligands showed the gradual changes of fluorescent color with reversibility from 4 K. [7-10] The unique color-changing behavior is ascribed to the temperature-dependent energy transfer efficiency. The thermochromic visible color variation around 90 K was reported on salicylideneaniline derivatives. [11-13] The temperaturedependent tautomerization of the two forms proceeds during the color changes in the solid crystalline state. The similar color changes were observed on a solidstate conjugated polymer, namely poly(3dodecylthiophene), in the range of 110-420 K. [14] As the ratio of two conformations varies depending on temperature, the intensity of the two peaks in the absorption spectra shows the ratiometric changes. However, the gradua...