Extraction of photosynthetic electrons from living plants or isolated photosynthetic complexes such as PSII, PSI, or thylakoids have recently been demonstrated. In particular, isolated thylakoids are stable and can be coated on various types of electrodes by simple drop casting or dip-coating methods. However, when the thylakoids coating become thicker, electrical connections are difficult to achieve between thylakoids and working electrodes. In this work, we propose use of carbon nanotubes (CNTs) to facilitate electrical connections between thylakoids and working electrodes. Thylakoids were extracted from spinach and different types of CNTs were prepared and added to the aqueous thylakoid solution. 1,2-dioleoyl-sn-glycero-3-phosphocholine (DOPC), Triton X-100, and mussel adhesive protein (MAP) were attached to CNTs and added to the thylakoid solutions. Zeta potentials of the three CNTs were measured and fluorescence responses of the CNTs were measured. The fluorescence quenching in MAP-treated CNTs and thylakoids solution as compared to thylakoids alone and the solution of CNTs treated DOPC or Triton X-100 and thylakoids suggests enhanced charge transfer between the thylakoids and the MAP-treated CNTs. Finally, photocurrent enhancement is demonstrated by measuring light-triggered currents from the MAP-treated CNT-thylakoid complexes.