A construct based on the electrostatic layer-by-layer self assembly technique has been fabricated, to be used as a tailored device to encourage nerve regeneration. A multilayered nanocoating composed of three precursor bilayers of cationic poly(dimethyldiallylammonium) chloride (PDDA) and anionic poly(styrenesulfonate) (PSS), followed by bilayers of poly-D-lysine (PDL) and antibody specific to transforming growth factor β1 (anti-TGF-β1), has been deposited on HYAFF 11®. The assembly process has been monitored by quartz crystal microbalance (QCM) for its characterisation and then it has been used on HYAFF 11®. Structural studies of the resulting multilayers confirmed stepwise deposition of anti-TGF-β1, with an average layer thickness of 2.2±0.2 nm and an average surface density of 0.36±0.03 μg cm−2. Scanning electron microscopy has been used to characterise multilayer uniformity. Finally, the immunological activity of the multilayered structure has been assessed. The results show that anti-TGF-β1 can be included in its active form in a predetermined multilayered structure onto HYAFF 11® with quantitative control of layer thickness and weight, providing a high tool with great potential in tissue engineering.