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We have made 53Cr NMR measurements on polycrystalline and single-crystalline film samples to study the local electronic state of a half-metallic ferromagnet CrO2 which has the rutile structure with one crystallographically equivalent Cr site. We observe two kinds of 53Cr NMR spectra in the ferromagnetic state of both the samples. An analysis on the hyperfine field shows the presence of two Cr sites with different orbital occupancies, suggesting that a local orbital order takes place with breaking the local symmetry in the rutile structure. This may be ascribed to the negative charge transfer between chromium and oxygen ions. [ABSTRACT FROM AUTHOR]