In this contribution, we report on the characterization of novel polyurethane graft-copolymers containing poly(n-butyl acrylate) side chains and, when extended, crystallizable polycaprolactone segments. Based on the previously reported synthesis, we attempt in the present work to correlate polymer structure and properties of segmented polyurethanes focussing on its potential interest as pressure-sensitive adhesive nanomaterial. For that purpose, thermomechanical analyses were coupled with complementary tack tests, rheology experiments and atomic force microscopy (AFM) imaging. Parameters such as relative hard and soft segments fraction or the. introduction of crystallisable fragments that can play an important role on the adhesive comportment are described as well.