Exploiting conductive biobased polymer nanocomposites for electromagnetic interference (EMI) shielding is a rapidly evolving research area. In this study, we systematically fine-tune the nano- and microstructural features of bacterial cellulose (BC) modified with poly(3,4-ethylenedioxythiophene) (PEDOT) for EMI shielding applications. First, to investigate the effect of nanostructure, PEDOT is incorporated into the BC matrix using two methods: chemical vapor polymerization (CVP) and