Surface modifi cation of biomaterials is a well-known
approach to enable an adequate biointerface between the
implant and the surrounding tissue, dictating the initial
acceptance or rejection of the implantable device. Since its
discovery in early 1990s layer-by-layer (LbL) approaches
have become a popular and attractive technique to
functionalize the biomaterials surface and also engineering
various types of objects such as capsules, hollow tubes, and
freestanding membranes in a controllable and versatile
manner. Such versatility enables the incorporation of
different nanostructured building blocks, including natural
biopolymers, which appear as promising biomimetic
multilayered systems due to their similarity to human
tissues. In this review, the potential of natural origin
polymer-based multilayers is highlighted in hopes of a
better understanding of the mechanisms behind its use as
building blocks of LbL assembly. A deep overview on the
recent progresses achieved in the design, fabrication, and
applications of natural origin multilayered films is provided.
Such films may lead to novel biomimetic approaches for
various biomedical applications, such as tissue engineering,
regenerative medicine, implantable devices, cell-based
biosensors, diagnostic systems, and basic cell biology.