The aim of this work was to prepare bioplastics, from renewable and biodegradable molecules, to be used as edible films. In particular, grass pea (Lathyrus sativus L.) flour was used as biopolymer source, the proteins of which were structurally modified by means of microbial transglutaminase, an enzyme able to catalyze isopeptide bonds between glutamines and lysines. We analyzed, by means of Zeta-potential, the flour suspension with the aim to determine which pH is more stable for the production of film-forming solutions. The bioplastics were produced by casting and they were characterized according to several technological properties. Optical analysis demonstrated that films cast in the presence of the microbial enzyme are more transparent compared to the untreated ones. Moreover, the visualization by scanning electron microscopy demonstrated that the enzyme-modified films possessed a more compact and homogeneous structure. Furthermore, the presence of microbial transglutaminase allowed to obtain film more mechanically resistant. Finally, digestion experiments under physiological conditions performed in order to obtain information useful for applying these novel biomaterials as carriers in the industrial field, indicated that the enzyme-treated coatings might allow the delivery of bioactive molecules in the gastro-intestinal tract.