With the rise of the plastic electronics, there has been a renewed interest in microstructure-sensitive design. Since processing conditions are known to heavily influence the microstructure, identifying optimal fabrication conditions is a crucial step towards the development of high-performance devices. A key component of this undertaking is the integration of effective computational tools; trial-and-error methods are no longer feasible, as they are time and resource intensive. In this work, several computational tools are developed to explore the process-structure-property relationships in designing high-performance thin film devices. More specifically, a phase-field -- based model, developed to simulate fabrication conditions, is coupled with advanced optimization routines to systematically identify promising processing conditions, in an automated way. Throughout this work, various processing conditions are explored and it is shown how they can be tuned to achieve the desired microstructure or device performance. The methodology presented here provides a scalable and extensible approach towards the rational design of tailored microstructures with enhanced functionalities.