Structurally anisotropic materials are ubiquitous in several application fields, yet their accurate optical characterization remains challenging due to the lack of general models linking their scattering coefficients to the macroscopic transport observables and the need to combine multiple measurements to retrieve their direction-dependent values. Here, we present an improved method for the experimental determination of light-transport tensor coefficients from the diffusive rates measured along all three directions, based on transient transmittance measurements and a generalized Monte Carlo model. We apply our method to the characterization of light-transport properties in two common anisotropic materials—polytetrafluoroethylene tape and paper—highlighting the magnitude of systematic deviations that are typically incurred when neglecting anisotropy.