In the past several years, polymer-fullerene mixtures have been intensely studied for use in organic solar cells because they can be deposited from solution, are compatible with lowcost roll-to-roll fabrication technology, and have shown high power conversion efficiency (g), up to 4-5%. [1][2][3] The best devices consist of a single bulk-heterojunction active layer, in which the polymer (donor) and fullerene (acceptor) are deposited from a common solvent. As the solvent dries the donor and acceptor components separate into domains. The final efficiency of the solar cell has been shown to be extremely sensitive to the size, composition, and crystallinity of the formed domains. [4,5] Improvement of the morphology in devices fabricated with a mixture of [6,6]-phenyl C 61 -butyric acid methyl ester (PCBM) and regioregular poly(3-hexylthiophene) (P3HT) has been achieved by using heat-treatment techniques [2,6] and long-time solvent curing, [1] with resulting record efficiencies. More recently, a method for increasing the crystallinity of the P3HT component has been introduced which involves filtering preformed nanofibers of P3HT out of solution and mixing the prepared nanofiber dispersion with PCBM to increase the efficiency of as-cast devices. [7] Interestingly, the best device performance was achieved by mixing lower-molecular-weight (M W ) amorphous P3HT back into the solution to reduce the crystalline content of the active layer and, thereby, to increase connection between crystalline domains. Studies of the M W impact on P3HT/PCBM solar cells have indicated that a large polydispersity and number-average molecular weight (M n ) over 19000 g mol -1 leads to improved efficiency. [8,9] Morphology studies of organic field-effect transistor (OFET) devices indicate that the increased M W leads to better network formation between crystalline domains. [10,11]