Electrospinning provides a promising route to quickly produce high-purity ceramic fibers from readily available sol-gel precursors. Recently, techniques have been developed to enable the production of biphasic nanocomposites on a single fiber, enabling the development of novel composites with connectivities that are difficult to obtain using existing methods. These composites on a fiber can be used as a unique anisotropic building block for creating more complex ordered structures. This work examines links between processing, structure, and properties for Janus-type composite nanofibers for the magnetoelectric BaTiO3-CoFe2O4 system. Specifically, we show how altering the viscosity and conductivity of precursor solutions can provide a unique route to synthesize biphasic composites of a range of sizes and compositions. Furthermore, we show how altering these properties can impact the magnetic and magnetoelectric behavior of these fibers. While this work focuses specifically on the BaTiO3-CoFe2O4 system, lessons learned can be applied to electrospinning biphasic ceramic materials from a variety of material systems and applications.