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Optimizing the properties of electrospun polymer-perovskite nanofibers is considered essential for improving the performance of flexible optoelectronic devices. Here, the influence of electrospinning setup parameters (i.e., electrical voltage, collector type (planar or rotary), rotation speed, as well as process time) on the properties (i.e., external structure, perovskite crystallinity, optical properties, thermal properties, the shrinkage ratio, mechanical properties, and long-term stability) of electrospun polyvinylpyrrolidone nanofibers modified with cesium lead iodide nanocrystals has been studied. The results have shown that the structure of nanofibers is related to the electrical voltage, collector rotation speed, and process duration. Perovskite crystallinity and light absorption have improved by increasing the electrical voltage or/and the process time. The polymer’s glass transition temperature is affected by the embedded perovskite and the collector’s rotation speed. The shrinkage ratio and mechanical properties of nanofibers have been controlled by the rotation speed and the electrical voltage. The shrinkage is caused by the stress created in the nanofibers during the electrospinning process. The best mechanical properties can be noticed with the rotary collector at a rotational speed of 500--750 rpm. Nanofibers have shown good long-term stability and high thermal stability. The long-term stability is inversely proportional to the value of the electrical voltage.