A new professional magnetic surfactant-based deep-eutectic (DE) and viscose liquefy catalyst (GS2+·2FeCl4, MGSFe) was synthesized by an optimized reaction of the as-prepared cationic gemini-surfactant (GS) with two moles of FeCl3·6H2O. The structure of the GS and MGSFe were characterized by NMR, FT-IR, UV–visible, CHN, pH, surface tension (ᵞ), and vibrating sample magnetometry (VSM) analyses. The MGSFe, that is a high viscose brownish liquid at >50 °C, was successfully tested as a highly active paramagnetic catalyst for improved benzoin condensation and three-component synthesis of substituted pyrroles with the highest turnover number (TON) and turnover frequency (TOF) that ever reported for this purpose. The superior activity of MGSFe is due to its amphiphile properties, the synergistic effects between GS2+ and 2FeCl4− as hydrogen-bond-donor and magnetic hydrogen-bond-acceptor components of this novel magneto-responsive DE, and reusability without loss of activity even in four consequence cycles run for synthesis of pyrroles. This magnetic GS-based DE can be used as oil miscible additive, pollutant adsorbent, and carrier of biomaterials to targeted poisons.