Catalytic hydrodeoxygenation (HDO) of phenolics to aromatics is one of the most important reaction routes in bio-oil upgrading. Sulfided CoMo catalysts are good candidates for this reaction, but their activities are strongly associated with the number of exposed surface sites and Co-Mo synergy. Herein, we employ zeolitic imidazolate framework-67 as a cobalt precursor and template for inverse deposition of MoS2 ultrathin sheets inside the framework to form CoMoS interfaces by using a simple hydrothermal method. The size-confined MoS2 possesses a fewlayered structure and abundant surface defects. It is found that in situ generation of a CoMoS active phase would take place to reach the best activity of our catalysts under the HDO reaction condition or by H-2 prereduction treatment. With varying different Co-Mo molar ratios, the optimized CoMoS-0.18 catalyst exhibits the highest HDO activity, with a p-cresol conversion of 92.4% and a toluene selectivity of 95.5% at 250 degrees C. The high performance is ascribed to the formation of an accessible surface CoMoS phase after surface restructuring.