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Abstract Using microwave irradiation, PtCo alloy nanoparticles were deposited within a few minutes on COOH‐functionalized MWCNT supports. The obtained catalysts were used for selective hydrogenation of cinnamaldehyde, a reaction whose products are widely used in various fields. In the selective cinnamaldehyde hydrogenation to cinnamyl alcohol, microwave‐prepared catalysts (generically, Pt_xCo_y‐MW) outperformed a catalyst prepared by the conventional method (Pt₁Co₂‐con). The highest selective hydrogenation to cinnamyl alcohol, 89%, was obtained using Pt₁Co₂‐MW, while Pt₁Co₂‐con showed a selectivity of 76%. Characterization results confirmed that the microwave prepared samples had a stronger interaction between Pt and Co than that in the Pt₁Co₂‐con sample. The alloyed Co altered the electronic structure of Pt, leading to favorable adsorption of the C=O bond by the lone‐pair electrons of its oxygen atom. Moreover, the Pt₁Co₂‐MW sample showed neglectable change in catalytic performance (e. g., cinnamaldehyde conversion and selective hydrogenation to cinnamyl alcohol) during recycling experiments.