Alcohol dehydrogenation to carbonyl compounds and hydrogen (H2) gas offers a green and sustainable method for producing H2 and the synthesis of various pharmaceuticals and fine chemicals. However, it is a challenge to acquire remarkable selectivity toward carbonyl products. Herein, [email protected] catalyst displays high dehydrogenation over dehydration reaction for isopropanol. [email protected] core–shell was synthesized from the carbonization of metal–organic frameworks (MOFs) via a single step without the need for incorporating an external source of carbon. [email protected] showed high selectivity (100%) and increased conversion (100%) of isopropanol to acetone and hydrogen via dehydrogenation. It exhibited high stability under the reactant flow for a long time and reusability for several cycles. A mechanism of the dehydrogenation was also highlighted using different analytical methods, including X-ray diffraction (XRD), electron diffraction (ED), Fourier transform infrared (FT-IR), and high-resolution transmission electron microscopy (HR-TEM).