As eries of MCM-41 supported metal catalysts (denoted M/ D41) were prepared by using the deep eutectic solvent( DES)mediated ionothermal synthesis strategy.A l/D41 was found to have excellent performance in the conversion of carbohydrates into 5-hydroxymethylfurfural (HMF). Furthermore, the production of HMF from glucose could be performed at high concentrationsincholine chloride aqueous solution (CAS;32wt%,relative to the reaction phase) and as ar esult, CAS is am ore promisings olventthan water and DES for HMF production.Biomass and carbohydrates are the focus of considerable attention for the production of valuable bio-based fuels and platform chemicals. [1] One particular bio-based platform chemical, 5-hydroxymethylfurfural( HMF),h as emerged as av ersatile chemicalf or the productiono fb iofuelsa nd fine chemicals. [2] However,t he conversiono fb iomass into HMF requires improvement if it is to be carriedo ut in quantities that can meet global demand. Without cost-effective HMF production routes, its full potential cannot be realized.HMF is generally obtained by the acid-catalyzed dehydration of carbohydrates. Previous studies have focused on homogeneous catalysts including mineral acids and metal-salts, but there are numerousi ssues associated with this strategy,s uch as equipment corrosion, environmental unfriendliness, and recycling difficulties. [3] The production of HMF has been examined by using heterogeneous catalysts that can be recovered and recycled, such as molecular sieves, [4] ion-exchange resins, [5] metal oxides, [6] and functionalizedm etal-organic frameworks. [7] However, the heterogeneously catalyzedc onversion of carbohydrates requires improvement;c urrent shortfalls include (1) low yields of HMF,( 2) low concentrations of the substrate, (3) excessive catalystr equirements, and (4) reduced activityo f the recycled catalyst. [8] Moreover,t he reaction media for the conversion of biomass into HMFh as to be carefully considered when targeting large-scale applications. Some recent reports concerned the use of water,p olar organic solvents, mixtures of water with organics olvents (biphasic [9] or singlep hase [10] ), ionic liquids, [11] and deep eutectics olvents (DESs) [12] for the production of HMF from carbohydrates. However,t he largescale potentialo ft hese strategies is hindered by side reactions (water), low conversion (polar organic solvents), toxicity/cost (ionic liquids), or low HMF yields (DESs). We recently reported that high HMF yields (> 90 %) are attainable from fructoseb y using aD ES (formed from choline chloride andf ructose) in the presence of al ow concentration of hydrochloric acid. [13] However,t his system is not suitable for heterogeneousc atalysis or the conversion of other carbohydrates or polysaccharides. We also found that renewable betaine-based catalysts in ag reen choline chloride (ChCl) aqueous solution (CAS)r eactionp hase led to enhanced yields of HMF from fructose. [14] In light of these prior studies, we set out to investigate CAS as ar eaction med...