Graphene oxide-silk composites have gained a significant interest in the recent times because of the unique mechanical properties of both GO and silk and their ability to form layered structures that exhibit a striking resemblance to the layered (brick-mortar) composites found in nature. However, various aspects of the interaction between silk and graphene oxide (e.g., conformation and distribution of the silk chains on chemically heterogeneous GO surface) are not completely understood. In this study, we demonstrate that the interaction between the silk fibroin chains and GO can be modulated by altering the pH of the silk fibroin solution. We employed atomic force microscopy (AFM) and Fourier transform infrared (FTIR) spectroscopy to probe the distribution and the secondary structure of silk fibroin adsorbed on GO. In acidic pH conditions (i.e., pH < pI), a high density of silk chains were found to adsorb on the GO surface, whereas an increase in pH resulted in a progressive decrease in the density of the adsorbed silk chains. This pH-dependent adsorption is ascribed to the electrostatic interactions between the negatively charged GO surface and the tunable ionization of the silk molecules. The secondary structure of silk fibroin chains adsorbed on GO was also found to be highly dependent on the pH. This study provides a deeper understanding of the interaction between GO and silk fibroin that is critical for the design and fabrication of bioinspired nanocomposites with tailored mechanical properties.