Wave-mode decomposition plays a very important role in elastic reverse time migration (ERTM). Improved imaging quality can be achieved due to reduced wave-mode crosstalk artifacts. The current state-of-the-art methods for anisotropic wavefield separation are based on either splitting model strategy, low-rank approximation, or lower-upper (LU) factorization. Most of these involve expensive matrix computation and Fourier transforms with strong model assumptions. Based on the anisotropic-Helmholtz (ani-Helmholtz) decomposition operator and decoupled formulations, we develop a novel and efficient P-/S-wave-mode vector decomposition method in vertical transverse isotropic (VTI) media with application in ERTM. We first review the basics of classical Helmholtz decomposition and isotropic decoupled formulations. In addition, the ani-Helmholtz decomposition operator is built from the P- and S-wave polarizations of the Christoffel equation in VTI media. We then derive novel decoupled formulations of anisotropic P-/S-waves based on the obtained ani-Helmholtz operator. Moreover, we use the first-order Taylor expansion to approximate the normalization term from the derived decoupled formulations and obtain an efficient ani-Helmholtz decomposition approach, which produces vector P- and S-wavefields with correct units, phases, and amplitudes. Compared with the previous studies, our approach mitigates model assumptions, avoids intricate calculations, such as LU factorization or low-rank approximation, and only needs three fast Fourier transforms at each time step. In addition, the graphic processing unit technique is used to dramatically accelerate various functions of ERTM, such as wavefields extrapolation, decomposition, and imaging. Three synthetic examples demonstrate the effectiveness and feasibility of our proposed approach.