Natural-abundance N-15 nuclear magnetic resonance (NMR) experiments show direct evidence for metal-pyridine interactions in blends of pyridine-containing polyurethanes and metal acetates. After blending with zinc acetate, the pyridine nitrogen peak shifts from -320 to -304 ppm; blending with magnesium acetate causes a shift to -309 ppm. Sodium acetate did not complex with the pyridine-containing polyurethanes; no shifts in the C-13 NMR signal for the acetate carbonyl or in the N-15 NMR for the pyridine nitrogen are apparent. Additionally, no interactions were evident for the urethane nitrogen site in any of the blends. Peak shifts, changes in cross-polarization dynamics, and increases in relaxation times were also apparent in the C-13 NMR spectra of the metal acetate-polymer blends. Effects of blending on the hard-domain hydrogen bonding were evident in FTIR and N-15 NMR contact-time experiments. The N-H stretching band shifted to higher wavenumbers and the N-15 NMR N-H signal persisted to longer contact times for the blend. Both spectroscopic techniques give evidence for complexation in these polyurethane blends.