A series of waterborne polyurethane (WBPU) adhesives were prepared with various ratios of aliphatic/aromatic diisocyanates, namely 4'-dicyclohexylmethane diisocyanate (H(12)MDI) as an aliphatic diisocyanate and 4,4'-diphenylmethane diisocyanate (MDI) as an aromatic diisocyanate with poly(tetramethyleneoxide-glycol) (PTMG), ethylene diamine (EDA) and dimethylol propionic acid (DMPA). (1)H-NMR spectroscopy was utilized to investigate the side reaction at the dispersion step during synthesis ofWBPU dispersions with respect to aliphatic, aromatic and mixed diisocyanates. The tensile strength, Young's modulus, elongation at break (%), storage modulus, glass transition temperature and adhesive strength were measured with respect to aliphatic/aromatic diisocyanate contents. The adhesive strength was maximum using mixed diisocyanates containing 25 mol% MDI in WBPU adhesives. (C) Koninklijke Brill NV, Leiden, 2011