Alginate-based hydrogels provide many advantages in the design of functional tissue mimetics given their low toxicity and mechanical similarities to native tissue types. However, deoxyribonucleic acid (DNA)-crosslinked alginate hydrogels are often not explored despite the added functional capabilities of DNA inclusion into the hydrogel. We have previously demonstrated the potential of DNA-encapsulated ionic alginate hydrogels to serve as human genetic training standards for forensic biology research and training. In this work, we present further development of these materials through covalent attachment of the DNA to alginate for targeted forensic applications. These crosslinked materials not only promote a more stable 3D polymeric network but also achieve localization of the functional ssDNA� which is particularly desirable for the development of human white blood cell (WBC) mimetics for forensic science. Herein, we investigated the covalent attachment of dual-amine-terminated ssDNA (N-DNA-N) to alginate of three different concentrations and various amine functionalities (none, one terminal amine, and two terminal amines). Fourier transform infrared spectroscopy analysis confirmed the formation of amide bonds, indicative of successful crosslinking between the N-DNA-N and alginate. Rheological characterization showed that each DNA-crosslinked material formed similar structures, but the higher DNA concentration behaved like a dynamic viscoelastic material. Scanning electron microscopy visualization indicated that each material had distinct topographies, where the covalent crosslinked alginate-DNA materials had more ordered particles and networked structures. It was revealed that the covalent crosslinking occurred primarily from the terminal amines on the DNA strands, further suggesting the formation of a 3D network. From here, microparticles (MPs) using dual-amine DNA-crosslinked materials were developed, and the particle morphology, sizes, and DNA functionality were assessed. It was determined that MPs made using DNA-crosslinked materials had larger particle diameters compared to non-DNA controls, and these MPs could be successfully processed in a relevant forensic scenario through extraction, amplification, and genotyping. The functionality of the DNA-crosslinked MPs demonstrates their feasibility for use as WBC mimetics that can be used as a standalone material and/or integrated into a forensic blood simulant containing genetic components.