Single-walled carbon nanotubes (SWNTs) have a set of unique mechanical and electrical properties that has stimulated tremendous interest in them. Significant efforts have been directed towards utilizing these materials as building blocks of composites for a variety of technological contexts, such as nanoelectronic devices, [1][2][3][4][5][6] sensors, [7][8][9][10][11][12] and field emission electron displays and lighting elements. [13,14] We strongly believe that one of the most prolific areas of their applications will be in biomedicine, where compact, strong, and high-performance devices can be engineered. These devices will exploit the properties of SWNTs and will compete with existing products. The novel technologies of diagnostics and therapeutics can be based on SWNT composites and individual tubes. Along these lines, SWNTs have been demonstrated as potential sensing materials of biological systems, [15][16][17][18][19] which are typically considered for the use in ex vivo modality. The potential use of SWNT-based structures for the purpose of healing neurological and brain-related injuries represents one of the major scientific and practical interests. The high mechanical strength and electrical properties possessed by SWNTs makes these materials perfect candidates for various prosthetic devices, including bone and joint repair. It is important to realize, however, that successful utilization of SWNT-based devices in biomedicine is hinged on the ability of such materials to interface with living cells, support their growth, and at the same time preserve their viability. [20][21][22][23][24] These factors are not well understood for any SWNT structures, which limits the development of in vivo, that is, implantable devices from such materials. The actual processes and techniques used for the preparation of macroscopic objects from SWNTs will play a significant role in determining cellular effects of SWNT composites. Substrates prepared from multi-walled carbon nanotubes (MWNTs) as well as SWNTs have been reported to be biocompatible platforms for neuronal growth and differentiation. [25][26][27] The use of carbon nanofiber composites as devices for neural-and bone-tissue-implant integration has also been described.[28] Molecular engineering of any SWNT-based composite should have a great effect on how the material performs during long-term contact with tissue. The layer-by-layer (LBL) approach to prepare SWNT structures can be particularly useful in this respect because it allows one to exert control over the structure of the SWNT/polymer systems from angstrom to nanometer and micrometer scale, which is necessity for the engineering of the cell/SWNT interface. [29] Recently, we demonstrated that SWNT LBL films can support the growth, viability, and differentiation of neuronal NG108-15 neuroblastoma/glioma hybrid cells. [30] The first example of free-standing SWNT/polymer thin-film membranes that can be mechanically compatible with tissues and can be used as implants and repair devices for neurological-or bra...