The controllable synthesis of materials with the desired structure and dimensionality is of great significance in material science. In this work, the hierarchical CNTs/Fe3O4@copper silicate(CNTs/Fe3O4@CuSilicate) composites was synthesized via a simple chemical conversion route by using CNTs/Fe3O4@SiO2 nanocables as template. Firstly, magnetic CNTs composites (CNTs/Fe3O4) were synthesized by the high temperature decomposition process using the iron acetylacetonate as raw materials. Then a layer of SiO2 can be easily coated on the magnetic CNTs by the stöber method, which were then converted into CNTs/Fe3O4@CuSilicate composites by hydrothermal reaction between the silica shell and copper ions in alkaline solution. The resulting CNTs/Fe3O4@CuSilicate composites hold merits such as magnetic responsivity, good dispersibility, and large specific surface area. Moreover, the CNTs/Fe3O4@copper silicate composites have strong affinity toward bovine hemoglobin(BHb), which were successfully applied to convenient, efficient, and fast removal of abundant proteins(HHb and HSA) in human blood.