The selective hydrogenation has attracted increasing attention to chemists for the production of value‐added products in chemical industry. Over the past several decades, substantial effort has been devoted to the design of catalyst for the selective hydrogenation of light alkynes and α, β‐unsaturated aldehydes, two classic cases for selective hydrogenation in chemical industry. Despite the great progress, it remains great challenges to achieve the selective hydrogenation because the desired products are generally thermodynamically unfavored. Here, we summarize the recent advances on selective hydrogenation using noble metal nanocrystals, with an emphasis on the surface engineering of noble metal nanocrystals for the selective hydrogenation of light alkynes and α, β‐unsaturated aldehydes. We will highlight the strategies for surface engineering, the advanced techniques for characterizations, as well as mechanism studies. We hope this review will promote chemists to develop efficient and robust catalysts for selective hydrogenation.