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The catalytic dehydrogenation of readily available alcohols to high value‐added carbonyl compounds is a research hotspot with scientific significance. Most of the current research about this reaction is performed with noble metal‐based homogeneous catalysts of high price and poor reusability. Herein, highly dispersed Co‐cluster‐decorated N‐doped carbon nanotubes (Co/N‐CNTs) were fabricated via a facile strategy and used for the dehydrogenation of alcohols with high efficiency. Various characterization techniques confirmed the presence of metallic Co clusters with almost atomic dispersion, and the N‐doped carbon supports also enhanced the catalytic activity of Co clusters in the dehydrogenation reaction. Aldehydes as dehydrogenation products were further transformed in situ to carboxylic acids through a Cannizzaro‐type pathway under alkaline conditions. The reaction pathway of the dehydrogenation of alcohols was clearly confirmed by theoretical calculations. This work should provide an effective and simple approach for the accurate design and synthesis of small Co‐clusters catalysts for the efficient dehydrogenation‐based transformation of alcohols to carboxylic acids under mild reaction conditions.