Understanding the deformation mechanism of amorphous polymeric materials is indispensable for their applications but is quite challenging. Here, with amorphous plasticized poly(vinyl butyral) (PVB) as a model system, we studied its structural change in situ during uniaxial deformation with ultrasmall-angle X-ray scattering (USAXS). We observed a stretch-induced phase separation behavior characterized by a butterfly scattering pattern in plasticized PVB for the first time. This phase separation, featured by a concentration fluctuation along the stretch direction, is a result of stress–concentration coupling under stretch. The phase size at its formation is around 100 nm, which increases almost linearly with strain. The strain rate has a weak effect on the phase size. This suggests that the elastic deformation of the network, cross-linked by entanglements and hydrogen-bonding clusters, governs the phase size. We proposed a tentative model to explain the deformation behavior of plasticized PVB, where the breaking and reforming of hydrogen bonds, the formation and growth of phase separation against osmotic pressure, and the plastic deformation and rupture of phase structure dissipate a large amount of energy and endow the plasticized PVB with excellent mechanical performance. We believe our findings are general and should be applicable to other amorphous polymers with solvents or plasticizers.

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As a key component in laminated glass, plasticized polyvinyl butyral (PVB) interlayer is a kind of impact‐resistant polymer material with high toughness. Recently, by using ultrasmall angle X‐ray scattering (USAXS) technique, Stretch‐induced phase‐separated structure on the scale of hundreds of nanometers formed in plasticized PVB for the first time is reported. In this work, the multiscale relaxation behavior of plasticized PVB is further investigated. The relaxation behavior of deformed plasticized PVB is studied from macroscopic stress, mesoscopic phase‐separated structure, and microscopic chain segment by combining USAXS, and birefringence with in situ stretching device. The contributions of chain segments and hydrogen bonding clusters for the multiscale relaxation behavior are discussed.