Magnetic polypyrrole-gelatin-barium ferrite (PPy-G-BaFe) cryogels/aerogels were synthesized by one-step oxidative cryopolymerization of pyrrole in the presence of various fractions of barium ferrite (BaFe) nanoparticles, dispersed in aqueous gelatin solution. The successful incorporation of BaFe into the composites was confirmed by elemental analysis and scanning electron microscopy paired with an energy-dispersive X-ray detector. The maximum achieved content of BaFe in the resulting material was 3.9 wt%. The aerogels with incorporated BaFe had significantly higher specific surface area and conductivity, reaching 19.3 m2 g-1 and 4 × 10-4 S cm-1, respectively, compared to PPy-G aerogel, prepared in the absence of BaFe (7.3 m2 g-1 and 1 × 10-5 S cm-1). The model adsorption experiment using an anionic dye, Reactive Black 5, showed that magnetic PPy-G-BaFe aerogel, prepared at 10 wt% BaFe fraction, had significantly higher adsorption rate and higher adsorption capacity, compared to PPy-G (dye removal fraction 99.6% and 89.1%, respectively, after 23 h). Therefore, the prepared PPy-G-BaFe aerogels are attractive adsorbents for water purification due to their enhanced adsorption performance and the possibility of facilitated separation from solution by a magnetic field.