Layer-by-layer (LBL) assembly has been widely utilized for constructing functional coatings to fabricate versatile materials. However, challenges arise when the assembly building blocks are electrically neutral. To address this issue, we report the use of mussel-inspired adhesion as a unique driving force for LBL assembly to fabricate electrically conductive cotton fabric (ECCF) with carbon nanotubes & graphene as conductive materials and poly(vinyl alcohol-graft-3,4-dihydroxybenzyl acetal) (PVD) as a mussel-inspired adhesive. The robust adhesion provided by PVD endowed the ECCF with excellent stability against sandpaper friction, tape peeling, and water washing. The use of the ECCF in some advanced application such as strain sensing, temperature sensing, and electric heating was studied in detail. The ECCF exhibited fast response and remarkable sensitivity in strain sensing, enabling real-time detection of various human motions such as bending, twisting, and swallowing. In temperature sensing, the ECCF exhibited a negative temperature coefficient effect and offered a linear response within the temperature range of 30–100 °C. In addition, the ECCF demonstrated exceptional electric heating performance, leading to potential use in outdoor insulation and thermal rehabilitation therapy. This innovative application of mussel-inspired adhesion in LBL assembly not only paves the way for advanced smart fabrics but also enhances functionality.