Platinum (Pt) -free counter electrodes (CEs) for dye sensitized solar cells (DSSCs) were developed using freestanding flexible single wall carbon nanotube (SWNT) films called bucky papers (BPs). BP was irradiated with microwave plasma, created using a mixture of Ar (1%) and H₂ (99%) gases, for 2 h. Raman scattering measurements revealed that no significant defects were created in the SWNTs as a result of the treatment. Plasma-treated BP (P-BP) developed vertically oriented, micron sized, pillar-like structures on its surface, while its base was still a dense random mesh of SWNTs. This unique flexible film had a larger accessible surface area and better catalytic properties. The plasma treatment improved the efficiency of BP-based DSSCs from 2.44% to 4.02%, which is comparable to Pt thin film (4.08%). The P-BP based solar cell operated with an open circuit voltage of 0.73 V and a fill factor of 0.70. It also had much higher efficiencies than films of randomly oriented plasma treated SWNTs. Using electrochemical impedance spectroscopy, the charge transfer resistances of P-BP and Pt were found to be 1.46 and 1.73 Ω cm², respectively.