The miscibility of polyester/nitrocellulose blends was investigated by differential scanning calorimetry and Fourier‐transform infrared (FTIR) spectroscopy. Two nitrocelluloses (NC) derived from wood and having different nitrogen contents (12.62 and 13.42%) were used. On the basis of the glass transition temperature criterion, poly(ϵ‐caprolactone) (PCL), poly(valerolactone), poly(ethylene adipate), and poly(butylene adipate) are miscible with nitrocellulose, whereas poly(α‐methyl α‐propyl β‐propiolactone) and poly(α‐methyl β‐proiolactone) are immiscible. The Tg versus composition curves of PCL/NC blends do not follow a monotone function but exhibit a singular point at a critical PCL volume fraction of 0.51 for NC‐1342 and 0.45 for NC‐1262 in agreement with Kovacs' theory. A shift of 17 cm‐1 of the carbonyl stretching band was observed with PCL/NC blends and is taken as evidence for hydrogen bonding interaction between the PCL carbonyl group and NC hydroxyl group. The frequency difference between the free hydroxyl absorbance and the absorbances of the hydrogen‐bonded species was found to be 85 cm‐1 in pure NC and 125 cm‐1 in PCL/NC blends; it indicates that the average strength of this interaction is stronger than the corresponding self‐associated hydrogen bonding in pure NC. The presence of a dipole‐dipole interaction between the nitrate‐ester groups of NC and the carbonyl groups of the polyesters is reported. The relative strength of the hydrogen bonding and dipole‐dipole interactions is discussed and correlated with polymer miscibility.

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