Valleytronic devices in which both the encoding and processing of information are achieved by manipulating electronic valley degrees of freedom are drawing increasing interest. However, materials with sizable intrinsic valley polarization are currently very rare. Using first‐principles calculations, a promising 2D multiferroic CuCrP 2 Te 6 monolayer with intrinsic valley and spin polarization is proposed. The valley splitting at the corners of the Brillouin zone (K and K′) with opposite Berry curvatures can be as large as 110.4 meV, which is quite promising for achieving an anomalous valley Hall effect. Moreover, such valley splitting can be tuned through different approaches, such as modulating the spin polarization and electric polarization and external strain. The interplay between valley and multiferroic properties reveled herein offers a unique strategy for the valleytronic device applications.