LAUSR

This article reports a three‐step process: 1) the hydrogenation of phenol, 2) aldol condensation between the cyclohexanone produced in reaction 1 and an aldehyde, and 3) hydrogenation of the aldol reaction product. This is achieved using palladium containing supported dendrons for reactions 1 and 3 and non‐metal containing supported dendrons for reaction 2. Palladium/dendron‐OMS catalyzes the phenol hydrogenation with a cyclohexanol yield of 85 %, the parent dendrons (no Pd) catalyze the Aldol reaction with over 80 % yield in some cases, and the Pd‐dendron samples can be used to hydrogenate the aldol coupling product at high yields, not dissimilar from what one observes from aqueous phase reforming (APR). The operating conditions of low temperature and low‐pressure hydrogen in aqueous media are consistent with green chemistry goals.