Reflecting light to a predetermined nonspecular direction is an important ability of metasurfaces, which is the basis for a wide range of applications (e.g., beam steering/splitting and imaging). However, anomalous reflection with 100% efficiency has not been achieved at optical frequencies yet, because of losses and/or insufficient nonlocal control of light waves. Here, we propose an all-dielectric quasi–three-dimensional subwavelength structure, consisting of multilayer films and metagratings, to achieve perfect anomalous reflections at optical frequencies. A complex multiple scattering process was stimulated by effectively coupling different Bloch waves and propagating waves, thus offering the metasystem the desired nonlocal control on light waves required by perfect anomalous reflections. Two perfect anomalous reflectors were demonstrated to reflect normally incident 1550-nm light to the 40°/75° directions with absolute efficiencies of 99%/99% in design (98%/88% in experiment). Our results pave the way toward realizing optical metadevices with desired high efficiencies in realistic applications.