Plastics are good examples of the "take-make-waste" production model, with the vast majority of its production coming from fossil petrochemical feedstocks and most of its disposal relying on landfilling or incineration. These practices lead to severe, negative environmental and economic impacts due to their accumulation and biodegradation recalcitrance. Due to the non-renewable origin of plastics, such a paradigm also raises questions about its scarcity and potential impact on production chains worldwide in the near future. Polyethylene terephthalate (PET) is one of the most single-used plastics produced worldwide, with wide applicability in the textile fiber and packing industries. The most common recycling process applied to PET is mechanical grinding followed by melting and reforming. Such processes lead to a downcycling: each cycle produces a material with fewer mechanical properties of interest, which eventually hampers further recycling. In recent years, plastic recycling research has gained new momentum with the identification of a PET hydrolase isolated from I. sakaiensis capable of degrading PET close to room temperature. Many other PET hydrolases have been characterized since then, improving catalysis rates, enzyme thermostability, and reaction conditions. Still, most enzymatic protocols struggle with degrading high-crystallinity substrate or performing well under low-pH conditions, which are the main challenges in reducing the cost of enzymatic PET degradation. More recently, molecular dynamics (MD) simulations have provided many structural insights into the interactions between PET and many different esterases. In addition, other studies have modeled the interaction between carbohydrate-binding modules and PET crystal films to understand the forces driving such interactions, aiming to improve the binding of PET hydrolases onto high-crystallinity regions of PET. At the core of those studies, force field parameters modeling PET nonbonded interactions will determine the accuracy of any prediction. Current force field models available for PET do not capture the complex electronic polarization effects of PET residues, which likely influence the behavior of PET in specific electronic microenvironments, such as enzyme active sites or at PET-solvent interfaces.