studies ignored the crucial role of the amorphous phase in delivering required force and chain tension into the crystalline phase in order to disintegrate it, and mainly focused on modeling the stressstrain curves or characterize the changes in crystalline structure. [8-13] However, the right strategy to tackle this elusive problem, i.e., molecular mechanics of semicrystalline polymers, should be a bottom up approach that first understands melt rheology and molecular mechanics of pure glassy phase and in the next stage by incorporating crystalline phase into the disordered phase tries to perceive the effects of crystalline phase on the mechanical performance of the resultant composite system. In this regard, study of semicrystalline polymers with higher T g than room temperature such as polyesters; e.g., poly(l-lactic acid) (PLLA) and poly(ethylene terephthalate) (PET), could be more useful in providing suitable model polymers that are able to be quenched below T g and produce amorphous counterparts as control samples. Another benefit with these polymers is that we are able to easily study the mechanical behavior both below and above T g. Previous studies by Flory [14] and Peterlin [15,16] tried to understand the yielding of semicrystalline polymers by characterizing the changes of crystalline phase in presence of stress. More recent studies by Strobl [17,18] on semicrystalline polymers with high T g treated the crystalline phase as a force-transmitting skeleton. Unlike preceding studies, the objective of this paper is to understand the semicrystalline state as a composite structure of amorphous and crystalline phases by focusing on the imperative role of amorphous phase in connecting crystalline regions to one another and providing local stress exerted on crystalline regions to cause yielding to occur in the crystalline phase. The importance of chain networking in amorphous phase, and interaction of amorphous phase with crystalline phase in delivering mechanical input into crystalline regions are highlighted in our study. Based on the new framework, for the first time, to the best of authors′ knowledge, the brittle response of a semicrystalline polymer under compression deformation is predicted and experimentally demonstrated in this study. We demonstrate that the effective deformation of crystalline phase is impossible in absence of a robust amorphous phase. In other words, based on our results that is the amorphous phase, which its deformation generates Different semicrystalline polymers including poly(l-lactic acid), poly(ethylene terephthalate), syndiotactic polystyrene, and polyamide 12 are studied in terms of their mechanical response to uniaxial compression deformation. Apparent decoupling of yielding of amorphous and crystalline phases is identified as separate peaks in the stress-strain curve in the vicinity of the glass transition temperature. The same feature is also observed for the uniaxial extension of predrawn semicrystalline poly(ethylene terephthalate). It is indicated that in absence of a stron...