Carbonation and chloride ions are known to be the two major factors responsible for the premature corrosion of steel reinforcement in concrete. Surface coatings on concrete can provide an effective and efficient protection for both concrete and the steel embedded in it, and can enhance the long-term durability of concrete materials and concrete structures exposed to aggressive environments. In practice, concrete is often cracked, and the crack-bridging ability of coatings is an important factor to be considered in evaluating their performance characteristics. Four different surface coatings were evaluated for their crack-bridging ability by tests of exposure to ozone and ultraviolet light, and for their ability to control chloride penetration and steel protection by accelerated wet-dry or continuous salt spray tests. From these results, a highly elastic acrylic rubber coating was chosen for further long-term stability tests. The data presented show conclusively that the acrylic rubber coating can prevent penetration of water, air and chloride ions, and ensure the long-term durability of steel embedded in concrete both when the concrete is free of chlorides and when it is contaminated with sodium chloride up to 1% of the mortar matrix. At high levels of chloride in the concrete, a high cover is also essential if the benefits of the surface coating are to be fully realized, and long-term serviceability of the concrete structure is to be ensured.