Grape fruit (Citrus paradisi Macf.) peel (GP) was used as raw material to prepare two novel biosorbents: CaGP (Ca2+ type) and MgGP (Mg2+ type). FTIR, SEM and N2 adsorption–desorption isotherms were used to characterize prepared adsorbents. Cd2+ biosorption by CaGP, MgGP and GP was investigated systematically by studying the effects of pH, biosorption time and initial concentration on the biosorption of Cd2+. The results showed that biosorption efficiencies of Cd2+ on CaGP and MgGP increased with increase in pH, and the highest removal of Cd2+ was occurred at pH 6.0. Meanwhile, Cd uptake capacity increased with contact time, and could reach equilibrium within 20 min. The rates of biosorption of Cd2+ on three prepared biosorbents were found to best-fit pseudo-second-order equation. Experimental isotherms were well fitted by Langmuir and Freundlich isotherms models. Moreover, according to the Langmuir equation, the maximum biosorption capacities (qm) of Cd2+ on CaGP and MgGP were found to be increased by 46.3% and 27.0%, respectively, compared with GP. The present study demonstrated that the waste grape fruit peel after simple Ca2+ or Mg2+ treatment could be used as a potential biosorbent for Cd2+, which indicated modified novel inactive/dead biological materials could remove Cd2+ from water.