The pumped storage power station (PSPS) is an important measure to achieve the strategic goal of “dual carbon”. As one of the preferred types for the upper reservoir dams of PSPSs, the concrete-faced rockfill dam (CFRD) often has a dam foundation on a steep transverse slop and is prone to produce slip deformation along the slope, resulting in poor anti-sliding stability of the dam slope. It is dangerous for the operation safety of PSPSs. Therefore, the slip deformation of CFRDs on dam foundations with large dip angles is investigated. The mechanism for the initiation of slip deformation is revealed. The design measures of physical mechanic and geometric structure are proposed to reduce slip deformation. The results show that the larger sliding forces and smaller anti-sliding forces are the fundamental reasons that CFRDs on dam foundations with large dip angles are prone to produce slip deformation. The larger the dip angle of the dam foundation, the larger the slip deformation of the dam body and face slab, and the smaller the safety factor of the dam slope. When the dip angle of the dam foundation is greater than 15°, the safety factor of the dam slope is less than the minimum value of 1.5 required by codes. The addition of pressure slopes can effectively reduce the slip deformation of the dam body or face slab and significantly improve the anti-sliding stability of the dam slope. When the height or width of the pressure slope platform is greater and the cohesion or internal friction angle of the pressure slope is larger, the slip deformations of the dam body and face slab are smaller, and the safety factor of the dam slope is greater. It is recommended that the height and width of the pressure slope platform be 1/2 times the maximum height of the main dam, and the density (cohesion and internal friction angle) of the pressure slope be equivalent to that of the main dam’s rockfill material. The research results can provide theoretical and technical support for the design and construction of CFRDs for the upper reservoir of PSPSs.