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The escalating environmental impact of pollution and the imperative to reduce carbon emissions have heightened the significance of developing biobased materials from natural biomass for electronic devices. This study investigates the utilization of biofermentation‐produced recombinant spider silk and animal‐derived hemin to create a novel biobased electret for field‐effect transistor memory. A critical challenge arises from the incompatibility between natural photoresponsive molecules and insulating biomaterials, resulting in severe phase separation that compromises film quality and morphology uniformity. This study systematically examines the effects of various film deposition and manufacturing techniques on the biobased electret's morphology, phase separation, and performance. Different methods demonstrate distinct advantages in terms of molecular aggregation/segregation, morphological homogeneity, and device performance. Phototransistor memory devices fabricated using spin coating and spray coating techniques exhibit robust aggregations and high memory windows of ≈30 V. Conversely, devices produced through solution shearing and electrospinning methods display enhanced smooth morphologies and high photoresponsivity. The phototransistor memory comprising electrospun fibers holds the potential to achieve the highest memory ratio, reaching ≈105. These findings not only highlight the applications of biobased materials through scalable film deposition processes but also underscore the importance of refining their morphology, phase separation, and performance in optoelectronic devices. [ABSTRACT FROM AUTHOR]