A bacterial cellulose (BC) nanofibril network is modified with an electrically conductive polyvinylaniline/polyaniline (PVAN/PANI) bilayer for construction of potential electrochemical biosensors. This is accomplished through surface-initiated atom transfer radical polymerization of 4-vinylaniline, followed by in situ chemical oxidative polymerization of aniline. A uniform coverage of the BC nanofiber with 1D supramolecular PANI nanostructures is confirmed by Fourier transform infrared, X-ray diffractogram, and CHN elemental analysis. Cyclic voltammograms evince the switching in the electrochemical behavior of BC/PVAN/PANI nanocomposites from the redox peaks at 0.74 V, in the positive scan and at -0.70 V, in the reverse scan, (at 100 mV.s(-1) scan rate). From these redox peaks, PANI is the emeraldine form with the maximal electrical performance recorded, showing charge-transfer resistance as low as 21 Omega and capacitance as high as 39 mu F. The voltage-sensible nanocomposites can interact with neural stem cells isolated from the subventricular zone (SVZ) of the brain, through stimulation and characterization of differentiated SVZ cells into specialized and mature neurons with long neurites measuring up to 115 +/- 24 mu m length after 7 days of culture without visible signs of cytotoxic effects. The findings pave the path to the new effective nanobiosensor technologies for nerve regenerative medicine, which demands both electroactivity and biocompatibility.