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Funding Information: For financial support, Jukka Niskanen acknowledges the Department of Chemistry of the University of Montreal (Canada), and Jaana Vapaavuori is grateful for funding from Banting Postdoctoral Fellowship (Canada). Christian Pellerin acknowledges funding from the Natural Sciences and Engineering Research Council of Canada (NSERC #RGPIN‐2015‐04014). Dmitri Golberg is grateful to the Australian Research Council (ARC) for granting a Laureate Fellowship FL160100089 and Discovery project DP170100131. Publisher Copyright: © 2021 Wiley Periodicals LLC. Understanding interfacial interactions in polymer systems is crucial for their applicability for instance in adhesives and coatings. Enclosing polymers in a cylindrical volume provides a system for studying interactions dictated by a continuous interfacial layer and a bulk-like volume in the middle of the cylinders. Here, we describe a simple method for enclosing polymers into boron nitride nanotubes (BNNTs) and establishing the effect of the interfacial interactions on the glass transition temperature (Tg) of the polymers by infrared spectroscopy. The volume of the inner channel is large in comparison to the volume of the loaded polymer coils, allowing the polymer to expand along the inner channel, resulting in the effect of interfacial interactions on polymer dynamics dominating over confinement effects. As examples, we loaded poly(4-vinyl pyridine), poly(methyl methacrylate), poly(vinyl pyrrolidone), and poly(disperse red 1 acrylate) in BNNTs. The strongest interaction between the studied polymer and BNNTswas observed for poly(4-vinyl pyridine), which also caused a significant increase of Tg. In addition to characterizing the effect of interfacial interactions on the thermal transitions of the polymers, this method, which is generalizable to most soluble polymer materials, can be used for studying photoinduced transitions in photoactive polymers thanks to the transparency of the BNNTs at visible wavelengths.