In this study, we report a method for predictive, controlled, and highly aligned nanofiber production via Centrifugal Jet Spinning (CJS) using polycaprolactone (PCL) as a model polymer. We investigated the effects of fabrication conditions and their resulting dimensionless parameters, namely the Weber, Reynolds, and Capillary numbers, by correlating with fiber morphologies (fiber diameter, fiber alignment, bead frequency, bead aspect ratio, and scaffold porosity) and mechanical properties (linear modulus and ultimate tensile strength). We report a fabrication parameter lookup table based on the aforementioned dimensionless numbers, for the production of nanofiber scaffolds using the CJS. We built a scaled-up version of the CJS that uses a larger reservoir and successfully validated the reported lookup table for PCL as well as other polymers including polyethylene oxide, polylactic acid, and polyvinylpyrrolidone dissolved either in hexafluoroisopropanol or chloroform. We show that by carefully tailoring the polymer intrinsic properties and the Reynolds number, we can fabricate bead-free, continuous fibers. This method will allow other researchers to design and build their own CJS for the production of desired fiber scaffold networks by utilizing the appropriate dimensionless numbers for their system.