In this work, the catalytic hydrodeoxygenation of carvacrol, a model alkyl-phenolic compound representing alkylated bio-oils, was thoroughly investigated using Ni–Cu bimetallic catalysts supported on layered ITQ-2 zeolites. The ITQ-2 zeolite, characterized by its layered mesoporous and microporous architecture, was specifically selected due to its advantageous structure, providing enhanced accessibility and effective exposure of active catalytic sites. Systematic catalyst optimization was performed by varying the Ni:Cu ratio, adjusting zeolite pore structures, and methodically tuning reaction parameters including temperature (140–180 ℃) and hydrogen pressure (10–50 bar H2). Comprehensive catalytic performance testing identified the catalyst formulation of 4Ni–6Cu supported on ITQ-2 zeolite as optimal, achieving exceptionally high carvacrol conversions exceeding 90%, along with selectivities surpassing 80% toward fully deoxygenated hydrocarbons under relatively moderate reaction conditions (160 ℃, 40 bar H2). Extensive catalyst characterization techniques, including X-ray diffraction (XRD), temperature-programmed reduction (H2-TPR), and X-ray photoelectron spectroscopy (XPS), provided in-depth mechanistic insights. These analyses highlighted the preservation of zeolite structure post-metal deposition and identified significant synergistic interactions between Ni and Cu species, crucially facilitating enhanced reducibility and selective hydrogenation and deoxygenation activities. Notably, Cu incorporation significantly lowered the Ni reduction temperature, optimized metal dispersion, and activated hydrogen more efficiently, resulting in minimized side reactions and coke formation. Catalyst robustness and practicality were further validated using complex, real-world feedstocks, including alkylated guaiacol and actual alkylated bio-oils. Consistent catalytic activity, excellent product selectivity, and negligible deactivation after repeated reuse cycles underscored the catalyst’s effectiveness and feasibility for industrial-scale operations. Stability tests demonstrated that the catalyst maintained its high performance through multiple reaction cycles, and straightforward regeneration procedures effectively restored catalytic performance. Additionally, environmental and energy assessments revealed the optimized catalytic process substantially reduced waste production and energy consumption. Metrics such as energy-economic efficiency, environmental factor, environmental energy impact, and product carbon footprint were systematically evaluated, highlighting the economic viability and environmental sustainability of this catalytic approach. This research presents an effective and sustainable pathway for leveraging biomass resources, ultimately contributing to reduced carbon emissions in the aviation sector. The outcomes represent critical advancements toward scalable, economically viable, and environmentally sustainable processes for biomass-derived aviation fuels.