Abstract 5‐(Chloromethyl)furfural (CMF), a bio‐renewable chemical building block, has been produced in good isolated yields from biomass‐derived carbohydrates within a closed aqueous HCl‐1,2‐dichloroethane biphasic reactor in the presence of benzyltributylammonium chloride (BTBAC) as a phase transfer catalyst (PTC). The solvent‐economic, one‐pot strategy afforded CMF in 73% isolated yield (90 °C, 3 h) from sucrose with a combined yield of 84% for CMF and levulinic acid. The process was optimized on temperature, duration, solvent, type, and loading of PTC. Use of BTBAC led to nearly 10% increase in yield of CMF for all substrates when compared to control reactions.