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Abstract Utilizing Planck polarized dust emission maps at 353 GHz and large-area maps of the neutral hydrogen (Hi) cold neutral medium (CNM) fraction (f_CNM), we investigate the relationship between dust polarization fraction (p₃₅₃) andf_CNMin the diffuse high latitude ( $\left(b\right)>30°$) sky. We find that the correlation betweenp₃₅₃andf_CNMis qualitatively distinct from thep₃₅₃–Hicolumn density (N_Hi) relationship. At low column densities (N_Hi< 4 × 10²⁰cm⁻²) wherep₃₅₃andN_Hiare uncorrelated, there is a strong positivep₃₅₃–f_CNMcorrelation. We fit thep₃₅₃–f_CNMcorrelation with data-driven models to constrain the degree of magnetic field disorder between phases along the line of sight. We argue that an increased magnetic field disorder in the warm neutral medium (WNM) relative to the CNM best explains the positivep₃₅₃–f_CNMcorrelation in diffuse regions. Modeling the CNM-associated dust column as being maximally polarized, with a polarization fractionp_CNM∼ 0.2, we find that the best-fit mean polarization fraction in the WNM-associated dust column is 0.22p_CNM. The model further suggests that a significantf_CNM-correlated fraction of the non-CNM column (an additional 18.4% of the Himass on average) is also more magnetically ordered, and we speculate that the additional column is associated with the unstable medium. Our results constitute a new large-area constraint on the average relative disorder of magnetic fields between the neutral phases of the interstellar medium, and are consistent with the physical picture of a more magnetically aligned CNM column forming out of a disordered WNM.