In this study, novel magnetic nanoparticle (FeNi3) based gold NPs with high surface area and easy accessibility of active sites were successfully developed by a facile approach. FeNi3 was functionalized with ionic gelation (IG) groups acting as robust anchors so that the gold NPs were well dispersed on the FeNi3 without aggregation. Spirulina coating was carried out via a wet impregnation technique based on IG using tripolyphosphate as a cross‐linking agent. Because of the amplification effect of IG, high loading capacities were achieved for the nanocatalysts. Furthermore, FeNi3/IG/Au showed superparamagnetic properties, contributing to the easy recovery of the nanocatalysts by magnetic separation. FeNi3/IG/Au was developed for the synthesis of pyrazolopyrimidines in mild conditions. The FeNi3/IG/Au magnetic NPs were thoroughly characterized using transmission electron microscopy, field emission scanning electron microscopy, vibrating sample magnetometry, Fourier‐transform infrared spectroscopy, and thermogravimetric analysis. The FeNi3/IG/Au nanocatalyst showed high robustness and stability in reaction for up to five cycles without significant loss of activity, probably due to the high loading of IG in the catalyst.