Inorganic nanoparticles based on magnetite improve the mechanical, thermal, and magnetic properties of microporous cryogel polymer composites. Here we report the synthesis of microporous cryogel based on the crosslinked sodium vinyl sulfonate (Na-VS) and 2-acrylamido-2-methylpropane sulfonic acid sodium salt (Na-AMPS). The magnetite nanoparticles were inserted into Na-VS/Na-AMPS cryogel either during its crosslinking polymerization or by in-situ technique after its crosslinking. The morphology, particle sizes, thermal stability and magnetite contents of Na-VS/Na-AMPS cryogel and its magnetite composites were investigated. The prepared Na-VS/Na-AMPS cryogel and its magnetite composites were used as adsorbents for methylene blue (MB) cationic dye using optimum conditions. The magnetite Na-VS/Na-AMPS cryogel composite prepared by in-situ technique achieved the best adsorption MB removal capacity for 7 cycles among the other adsorbents via chemical adsorption mechanism at room temperature.