Electrospun ionic nonwovens are obtained by green electrospinning of aqueous dispersions. The resulting nonwovens are termed as chameleon nonwovens since their surface properties can be tailored in a large variety by coating of different functionalities following the protocol of the layer-by-layer process (LBL). The dimensional stability of the electrospun fibers in the chameleon nonwovens is achieved by photo-cross-linking after electrospinning and thereby overcoming the repulsive forces of the ionic moieties in the fibers. Depending on the nature of the ionic moieties different materials are coated by LBL including dyes, antibacterial materials, silver, and gold nanoparticles. Enhanced coating efficiency for coating of metal nanoparticles is observed when the chameleon nonwovens were precoated by a polyelectrolyte.