Green synthesis plays a crucial role in advancing sustainability within materials science. This study explores the integration of metal–organic frameworks (MOFs), obtained through green synthesis, using an electrospinning post-processing technique to develop MOF-based composite materials. The resulting novel multifunctional composites demonstrate enhanced stability and functionality, compared to their control counterparts. The integration of four types of MOFs into an electrospun fiber network was investigated using a specific polymer solution. Characterization and preliminary adsorption studies were conducted to elucidate the chemistry, morphology, and adsorptive capabilities of the resulting MOF composites. Electrospinning MOFs into polymer fibers improved their stability and dye removal capabilities. More specifically, optimization of MOF-to-polymer ratios and processing conditions yielded composites that are thermally stable, with modified surface area and porosity. Post-processing MOFs resulted in a fiber diameter increase of 44 and 109%, enhancing the composites by providing more MOF active sites and improved mechanical strength. Zirconium-based post-processed MOFs demonstrated superior dye removal, different from the copper-based dyes. Electrospinning technology has demonstrated significant potential in the fabrication of high-performance multifunctional MOF composites. This has helped to create advanced sustainable composites with tailored properties, paving the way for more targeted and efficient applications. The applications of these composites show promise for military engineering where durable, light weight, and multifunctional materials are critical in contributing to improved performance, operational efficiency, and safety.