AbstractSpintronics, micro/nanofabrication, and the semiconductor industry are undergoing significant transformations, highlighting the need for flexible technologie. This study examines the possibility of integrating topological insulators (TIs), specifically Bi2Te3 thin films (13–191 nm), into flexible spintronic applications through scalable magneto‐sputtering techniques, and investigates how structural organization influences electrical and topological properties through post‐thermal annealing. Films annealed above 250 °C display improved polycrystalline structure, larger crystallites, fewer local defects, and higher a room‐temperature Seebeck coefficient (S) and resistivity (ρ), suggesting decreased bulk electronic contributions. A metastable transport regime is identified in the temperature‐dependent resistivity of films annealed at 300 °C between 20–100 K; in this range, the thinnest film exhibits markedly metallic behavior, signaling the presence of topological surface states (TSS). Magnetoresistance measurements of as‐grown and annealed films, between 3–20 K, demonstrate weak antilocalization. Applying the Hikami‐Larkin‐Nagaoka model, α‐coefficients are found to scale with thickness from 0.5–1, indicating thickness‐controlled coupling of the TSS. Post‐annealing at 300 °C, the phase coherence length, Lϕ, of the thinner films increases, while the temperature dephasing rate shifts from ∼0.7 (as‐grown) to ∼0.5 (post‐annealing), aligning with expected values for 2D TSS. These are encouraging findings for large‐scale manufacturing flexible TI technologies, without sacrificing tunabilit.