Laser coatings are an enabling technology for laser systems. They are applied on the surfaces of most laser components. However, except for the intensity control of the light, laser coatings have limited capability to manipulate electromagnetic characteristics. Optical metasurfaces can locally manipulate optical fields and enhance light–matter interactions, thus offering fascinating possibilities to realize unprecedented photonic phenomena. As metasurfaces are further studied, efficiency becomes a bottleneck restricting laser application. Anomalous reflection is one of the most fundamental abilities of metasurfaces and is also the basis of many practical applications and complex operations. Therefore, realizing high-efficiency anomalous reflection is the benchmark problem to obtain optical metasurfaces with high efficiency. Taking advantage of the interplay between laser coatings and optical metasurfaces, it is possible to bring about a reform in high efficient multilayer-assisted-metasurfaces for laser applications. Multilayer-assisted-metasurfaces can realize functionalities and applications that are distinctly different from traditional laser components. In this talk, multilayer metasurfaces that exhibit abnormal reflection will be discussed with an outlook of potential applications for laser systems. Specifically, anomalous reflectors at 1550 nm were showcased in design by controlling the lateral energy flow generated by propagation wave via multilayer films. Fabrication and measurement were carried out to obtain the highest efficiency to confirm the validity of design methodology and structure. This paves the way towards high-efficiency optical metasurfaces and may promote the commercialization of optical metasurfaces.