Highlights To address the challenges of achieving strong adhesion between aluminum face sheets and composite cores (3D carbon felts) in sandwich structures, this work presents a novel approach that prioritizes safety, environmental sustainability, and ease of processing. The 3D CFs/Epoxy core was modified with Triton X‐100 in amounts from 0 to 10 wt% of the epoxy resin. The aluminum alloy face sheets were anodized at voltages from 0 to 11 V, using a NaCl‐based anodizing process. The technique of anodizing can enhance the bond between the aluminum face sheets and the 3D CFs/epoxy core, resulting in improved mechanical performance of the composite, including flexural and compressive testing, as well as dynamic mechanical analysis. The composite, embedding 3D CFs foam in epoxy resin, has a storage modulus 65.1% higher than pure epoxy at 2070 MPa. In addition, increasing Triton X‐100 content (1–10 wt%) decreases the storage modulus from 1886 to 1314 MPa and the glass transition temperature from 68.3 to 62.8 °C. Additionally, with Triton X‐100 concentrations of 1 to 10 wt%, the flexural modulus of the epoxy reinforced by 3D CFs drops from 3951.8 to 2400 MPa, and the flexural strength decreases by 55.3% from 174 to 112 MPa, indicating reduced structural rigidity. For sandwich composites with anodized aluminum face sheets, a 7 V anodizing voltage boosts the flexural modulus from 17.8 GPa (0 V) to 36.2 GPa. At 7 V, compressive strength and strain rise by 346.9% and 995.5%, respectively. Flexural toughness peaks at 11239 KJ/m3 with 5 wt% Triton X‐100. Developed new sandwich epoxy composites consisting of anodized aluminum sheet treated with NaCl and modified 3D carbon felts epoxy composites using Triton X‐100. Aluminum face sheets underwent an anodization at different voltages (0, 5, 7, 9, and 11 volts), aiming to enhance the bonding between the aluminum sheets and the 3D CFs/epoxy core. Triton X‐100 was utilized to modify the epoxy matrix at various concentrations (0 to 10 wt%) for improving the flexibility of the sandwich core. The sandwich composites incorporating the un‐anodized face sheet have shown flexural modulus of about 17.8 GPa. The modulus achieves its maximum value of 36.2 GPa when anodized at 7 V, indicating a 103% increase. The flexural strength of sandwich composites increases by 13% (272 MPa) when the Triton X‐100 concentration is raised to 5 wt%, compared to the 240 MPa flexural strength of the Al face sheet anodized at 7 V. [ABSTRACT FROM AUTHOR]