Valorisation of bio-oil to sustainable energy through hydrodeoxygenation process has been attracted much attention in the development of bio-refineries. The present work emphasizes on the development of a highly active heterogeneous catalyst for hydrodeoxygenation reaction with modified Laponite-gamma-alumina and SBA-15 - gamma-alumina composites as support for Mo and NiMo catalysts using Mo-inorganic -organic hybrid nanocrystals (HNCs) prepared under hydrothermal condition. The synthesized catalysts were characterised using N-2-physisorption, XRD, FT-IR, Raman, HRTEM, TPD/TPR, H-2 pulse chemisorption and XPS techniques. The catalysts were evaluated for HDO of eugenol (Lignin model compound, Clove oil) at 400 degrees C under atmospheric pressure. The physicochemical characterization of the support composites revealed that Mo-HNC supported on modified Laponite exhibited extraordinary stability, metal-support interaction and metal dispersion over the support. The catalytic activity results revealed that the Laponite composite supported NiMo-HNC catalyst performed complete conversion of eugenol with enhanced % selectivity to 3- and 4-propyl phenol (mono-deoxygenated products) and to benzene and 4-propyl cyclohexene (complete deoxygenated products). Thereby, a new Mo-HNC supported modified Laponite composite catalyst has been successfully developed. The role of the HNC-Mo preparation method, textural properties, morphology of Laponite composite catalysts have been demonstrated for efficient HDO of clove oil. (C) 2019 Elsevier Ltd. All rights reserved.