LiMnxCoyNi1−x−yO2 (LMCNO) has been broadly investigated and commercialized primarily as lithium ion battery (LIB) cathodes, owing to its high operating voltage, large energy density, and superior electronic conductivity. However, poor cycling stability induced by the rapid structure degradation limits their further development. Coating is regarded as a very effective strategy to address the problem of structure degradation. Regrettably, the coating layers obtained by traditional methods are usually thick, which is not appropriate for delivering of integrated performance. As an emerging coating technology, atomic layer deposition (ALD) demonstrates immeasurable advantages in deposition of ultrathin coating materials because of its atomic-level precision, and has been widely applied in construction of the coating layers on LMCNO substrate materials. Herein, we firstly outline the development and mechanism of ALD technology, and then systematically summarize intrinsic reasons for the enhanced electrochemical performance. Finally, we propose new insights toward designing and preparing the coating structure of LMCNO cathodes by controllable ALD for the next-generation LIBs.