Although full-waveform inversion (FWI) has shown significant promise in reconstructing heterogeneous velocity fields, most existing methodologies are limited to acoustic models. We extend FWI to multicomponent (PP and PS) data from anisotropic media, with the current implementation limited to a stack of horizontal, homogeneous VTI (transversely isotropic with a vertical symmetry axis) layers. The algorithm is designed to estimate the interval vertical P- and S-wave velocities ([Formula: see text] and [Formula: see text]) and Thomsen parameters [Formula: see text] and [Formula: see text] from long-spread PP and PSV reflections. The forward-modeling operator is based on the anisotropic reflectivity technique, and the inversion is performed in the time domain using the gradient (Gauss-Newton) method. We employ nonhyperbolic semblance analysis and Dix-type equations to build the initial model. To identify the medium parameters constrained by the data, we perform eigenvalue/eigenvector decomposition of the approximate Hessian matrix for a VTI layer embedded between isotropic media. Analysis of the eigenvectors shows that the parameters [Formula: see text], [Formula: see text], [Formula: see text], and [Formula: see text] (density is assumed to be known) can be resolved not only by joint inversion of PP and PS data, but also with PP reflections alone. Although the inversion becomes more stable with increasing spreadlength-to-depth ([Formula: see text]) ratio, the parameters of the three-layer model are constrained even by PP data acquired on conventional spreads ([Formula: see text]). For multilayered VTI media, the sensitivity of the objective function to the interval parameters decreases with depth. Still, it is possible to resolve [Formula: see text], [Formula: see text], [Formula: see text], and [Formula: see text] for the deeper layers using PP-waves, if the ratio [Formula: see text] for the bottom of the layer reaches two. Mode-converted waves provide useful additional constraints for FWI, which become essential for smaller spreads. The insights gained here by examining horizontally layered models should help guide the inversion for heterogeneous TI media.