A microstrip air line system for measuring the complex permittivity of anisotropic materials in the band from 0.3 to 1 GHz is proposed. The multireflect-thru method is used to calibrate the measurement system in the whole band with a single microstrip air line without suffering from the limited space resolution of time-gating technique. During the measurement, the material under test (MUT) is placed both above and below the strip. With this deployment, the TEM mode propagates along the microstrip in the MUT. Therefore, it is possible to measure the anisotropic permittivity. Since a small portion of the electric field is parallel to the ground plane around two edges of the strip, the extracted property is not purely along one direction. To obtain higher accuracy, with the help of linear combination, the properties along two directions are disentangled by two measurements. For validation of the method, an isotropic material and an anisotropic material in the microstrip air line were simulated and their permittivities were extracted from simulation results. An anisotropic material polytetrafluoroethylene (PTFE) and two anisotropic materials, FR4 and honeycomb absorber, were measured. The results of PTFE show that there is a maximum relative error of 1.4% and 2.5% for the permittivity extracted from simulation and measurement, respectively. The validity and the accuracy of the system for measuring anisotropic materials are verified by the simulation and measurement results.