In our continuing quest to control the orientation of redox-active proteins on electrode surfaces, we have focused on chemical reactions at the lysine groups of Photosystem I while it is still part of the thylakoid membrane. The functionalization of protein complexes while still part of their native membrane can be confirmed by conventional analytical methods. After extraction of the now labeled stromal side of the photosystem I protein complex, we have explored a number of methods for achieving electron transfer directly through the orientated protein complex. These alternatives to direct chemisorption on surfce includes nanoparticle conjugation and other chemical reactions that take advantage of the chemical transformation on the stromal side. These advances will be detailed in this presentation.