Bacterial cellulose/oxidized bacterial cellulose nanofibrils (BC/oxBCNFs) macro‐fibers are developed as a novel scaffold for vascular tissue engineering. Utilizing a low‐speed rotary coagulation spinning technique and precise solvent control, macro‐fibers with a unique heterogeneous structure with dense surface and porous core are created. Enhanced by a polydopamine (PDA) coating, these macro‐fibers offer robust mechanical integrity, high biocompatibility, and excellent cell adhesion. When cultured with endothelial cells (ECs) and smooth muscle cells (SMCs), the macro‐fibers support healthy cell proliferation and exhibit a unique spiral SMC alignment, demonstrating their vascular suitability. This innovative strategy opens new avenues for advances in tissue engineering.