Chitin is the second most abundant biomass on earth but exploited the least. In this study, wastes from Uroteuthis duvauceli was utilized to extract 38.79 ± 1.38% dry weight of β-chitin using a new combination of decolorization, demineralization, and deproteinization processes. β-chitin was then derivatized with acrylamide in an efficient and green aqueous 8 wt% NaOH/4 wt% urea solvent via one-pot etherification. The success of carbamoylethyl ether of chitin and carboxyethyl chitin synthesis was confirmed by FTIR, 1H NMR, 13C NMR, XRD, SEM, TGA, and DSC. The synthesized acrylamide-modified β-chitin derivatives were shown to exhibit water solubility and lower decomposition temperatures, which are primarily due to the disruption of the crystalline structure of β-chitin upon its dissolution and modification. In this era of climate change, this desirable strategy of harnessing β-chitin from wastes and converting it to value-added products is highly sought to mitigate the continuing ecological and economical imbalance brought about by marine-food wastes. To the best of our knowledge, this novel contribution is the first to report biorefinery of squid pens from this particular species and functionalizing it with acrylamide in a facile manner, thus, offering greater potential for future development to biocompatible chitin-based biomaterials intended for industrial, pharmaceutical and biomedical applications.