This work investigates the temperature-responsive optical characteristics of vanadium oxide nanocrystals fabricated by plasma-enhanced atomic layer deposition (PEALD). Analysis of the films' absorption and ellipsoid spectra reveals a dual optical bandgap, linked to the evolving surface microstructure during film growth. Notably, variable-temperature absorption spectrum analysis shows these bandgaps respond differently to temperature shifts, revealing the microstructure's critical influence on optical performance. The research pioneers a novel method for tuning the optical properties of 2D vanadium oxide films through microstructural manipulation. This contributes to the scientific understanding and provides a foundation for developing functional films capable of dynamic dual-band light absorption regulation.