Mode-converted PS-waves can provide critically important information for velocity analysis in transversely isotropic (TI) media. We demonstrate, with physical-modeling data, that the combination of long-spread reflection traveltimes of PP- and PS-waves can be inverted for the parameters of a horizontal TI layer with a tilted symmetry axis. The 2D multicomponent reflection data are acquired over a phenolic sample manufactured to simulate the effective medium formed by steeply dipping fracture sets or shale layers. The reflection moveout of PS-waves in this model is asymmetric with respect to the source and receiver positions, and the moveout-asymmetry attributes play a crucial role in constraining the TI parameters. Applying the modified [Formula: see text] method to the PP and PS traveltimes recorded in the symmetry-axis plane, we compute the time and offset asymmetry attributes of the PS-waves along with the traveltimes of the pure SS reflections. The algorithm of Dewangan and Tsvankin is then used to invert the combination of the moveout attributes of PP-, SS-, and PS-waves for the medium parameters and the thickness of the sample. It should be emphasized that the pure-mode (PP and SS) traveltimes alone are insufficient for the inversion, even if 3D wide-azimuth data are available. Our estimates of the symmetry axis tilt and layer thickness almost coincide with the actual values. The inverted model is also validated by reproducing the results of transmission experiments with both P- and S-wave sources. The transmitted SV wavefield exhibits a prominent cusp (triplication) accurately predicted by the parameter-estimation results.