Alkali metals (lithium, sodium, and potassium) are promising as anodes in emerging rechargeable batteries, ascribed to their high capacity or abundance. Two commonly experienced issues, however, have hindered them from commercialization: the dendritic growth of alkali metals during plating and the formation of solid electrolyte interphase due to contact with liquid electrolytes. Many technical strategies have been developed for addressing these two issues in the past decades. Among them, atomic and molecular layer deposition (ALD and MLD) have been drawing more and more efforts, owing to a series of their unique capabilities. ALD and MLD enable a variety of inorganic, organic, and even inorganic-organic hybrid materials, featuring accurate nanoscale controllability, low process temperature, and extremely uniform and conformal coverage. Consequently, ALD and MLD have paved a novel route for tackling the issues of alkali metal anodes. In this review, we have made a thorough survey on surface coatings via ALD and MLD, and comparatively analyzed their effects on improving the safety and stability of alkali metal anodes. We expect that this article will help boost more efforts in exploring advanced surface coatings via ALD and MLD to successfully mitigate the issues of alkali metal anodes.