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Photocatalytic oxidation technology can mineralize hazardous volatile organic compounds (VOCs), but the poor photocatalytic oxidation activity limits its practical application. Here we develop Cu‐doped WO3 electrospun nanofibers through a non‐equivalent doping strategy. The Cu dopant prefers substituting five‐coordinated W atoms atop the WO3 matrix, inducing strong dopant/matrix interaction (SDMI) effect and prominent charge rearrangement. A localized electric field (LEF) forms pointing from positively charged WO3 matrix to negatively charged Cu dopant, which triggers efficient photoexcited charge separation. Further, the Cu dopant promoted the production of ⋅OH radicals and thereby enhanced VOCs photodegradation. The 0.7 % Cu‐doped WO3 nanofibers show optimal photocatalytic oxidation performance towards formaldehyde and acetone, 5.5 and 4.8 times higher than pristine WO3 nanofibers, respectively. This work highlights the role of dopant‐induced LEF on the charge carriers separation and might shed light on developing more efficient photocatalysts with non‐equivalent dopants. [ABSTRACT FROM AUTHOR]