The present work shows a procedure to valorize non-commercial boiled shrimp to produce functional ingredients, using a combined treatment based on enzymatic hydrolysis and subsequent glycation under mild conditions. Antioxidant and prolyl endopeptidase-inhibiting activities were determined as a function of hydrolysis and glycation times (0–120 min and 0–180 min, respectively). The reaction products were characterized by determining the degree of hydrolysis, browning, fluorescent compounds, free amino acids, phenol content, Fourier transform infrared spectroscopy (FTIR), and molecular weight of the different fractions obtained. Enzymatic hydrolysis generated hydrolysates with significant antioxidant and prolyl endopeptidase-inhibiting activities. Glycation under mild conditions was used as a strategy to improve the antioxidant and potential nootropic properties of the hydrolysates. During glycation, the free amino acid content decreased, total phenols and fluorescent compounds increased significantly, and low molecular weight melanoidins were formed. The presence of peptide-glucose conjugates was also confirmed by FTIR. Glycation increased the antioxidant activities of the hydrolysates; however, their prolyl-endopeptidase-inhibiting activity was lost. Results showed that compounds with promising antioxidant (hydrolysis and glycation) and potential nootropic (hydrolysis) activities and applications in food systems were obtained from the biotechnological strategy used.