Gold nanoparticles (AuNPs) coated with responsive polymers gained considerable interest due to their controllable size, good stability, and fast environmental response suitable for biological applications and sensing. Here we report on a simple and efficient method for the synthesis of stable and redox responsive AuNPs using organometallic polyelectrolytes in aqueous solutions of HAuCl4. In the redox reaction, positively or negatively charged poly(ferrocenylsilanes) (PFS+/PFS-) served as reducing agents, and also as stabilizing polymers. Due to their unique tunable electrostatic and electrosteric protection, AuNPs coated with PFS-, (PFS+)@AuNPs, possess high redox sensitivity, with reversible, repetitive, sustainable color switching between the assembled (purple color) and disassembled (red color) states as evidenced by UV-Vis absorption and TEM measurements. Feasibility studies reported here indicate that the particles described can be applied as a colorimetric probe for the detection of redox molecules, e.g. vitamin C, in a controlled and facile manner.