Perylene Diimides (PDIs) represent a special class of molecules that have gained interest in the areas of organic photovoltaics due to their physical properties such as near-unity fluorescence quantum yield, high photochemical stability and strong electron accepting character. Furthermore the physical properties of PDIs can be fine-tuned based on the substituents at the imide position of the molecule. Asymmetric PDIs containing two different substituents are highly desirable compounds due to their ability for example, to maintain good solubility while exhibiting additional chemical functionality for further modification. The issue at hand is that the yields for synthesis of such molecules are typically less than 10% using classical synthetic methods. The new method that we have developed has been shown to improve the yields of these molecules significantly (up to 42%) while also eliminating multiple synthetic steps. These results are critically important because it makes a wide variety of PDIs more readily available for further scientific progress in applications such as organic solar cells.