A strategy for the in line mass production of a three-dimensional (3D) non-woven nanofabric consisting of crystalline P3HT nanofibrils, created by in situ cooling of the transportation line to feed a P3HT solution for a coating tool, was introduced. The required cooling-temperature with respect to the feeding rate for the overall nanofibril creating process and the yield of the nanofibrils in solution with various organic solvents were determined. Considering the influence of a change in the temperature on the status of the precipitated nanofibrils until feeding it into the spray nozzle, the margin of the surviving nanofibrils at a certain temperature was also investigated. To verify the superiority of our strategy and present directions regarding its application to industry, arrays of organic solar cells based on a 3D non-woven nanofabric structure consisting of P3HT nanofibrils were designed and fabricated using our in situ process combined with a spray-coating system. As a result, through the in situ cooling process, a considerable solar energy harvesting efficiency near 4%, which is a state-of-the-art value in a bi-layer-based solar cell, was obtained.