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Extracellular matrix (ECM) is essential for tissue development, providing structural support and a microenvironment that is necessary for cells. As tissue engineering advances, there is a growing demand for ECM mimics. Polycaprolactone (PCL) is a commonly used synthetic polymer for ECM mimic materials. However, its biologically inactive surface limits its direct application in tissue engineering. Our study aimed to improve the biocompatibility of PCL by incorporating hemoglobin nanofibrils (HbFs) into PCL using an electrospinning technique. HbFs were formed from bovine hemoglobin (Hb) extracted from industrial byproducts and designed to offer PCL an improved cell adhesion property. The fabricated HbFs@PCL electrospun scaffold exhibits improved fibroblast adherence, proliferation, and deeper fibroblast infiltration into the scaffold compared with the pure PCL scaffold, indicating its potential to be an ECM mimic. This study represents the pioneering utilization of Hb-sourced nanofibrils in the electrospun PCL scaffolds for tissue engineering applications.