In this paper, a method was proposed to measure the elastic modulus of each layer-material in multi-layer cylindrical structures by OFDR in a large temperature range. Distributed measurement technology was used to carry out accurate measurements of strain distribution and numerical value on specimens. The accurate force-strain relationship can be obtained if the specimen is small or there is inevitable non-uniformity on the specimen. In this paper, a tensile test platform was built, and the tensile tests of optical fiber (−51.6 °C to 82.15 °C), polymer double-layer specimen (−54 °C to 63 °C), and composite three-layer specimen (−46 °C to 62 °C) were carried out. The elastic modulus of the three kinds of material and their relationships with temperature were obtained. By comparing with the standard test results, the accuracy and reliability of the test were verified.