This work reports highly selective phosphopeptide enrichment using amorphous TiO2 nanotubes (TiO2NTs) and the same material decorated with superparamagnetic Fe3O4 nanoparticles (TiO2NTs@Fe3O4NPs). TiO2NTs and TiO2NTs@Fe3O4NPs materials were applied for phosphopeptide enrichment both from a simple peptide mixture (tryptic digest of bovine serum albumin and α-casein) as well as from a complex peptide mixture (tryptic digest of Jurkat T cell lysate). The obtained enrichment efficiency and selectivi-ty for phosphopeptides of TiO2NTs and TiO2NTs@Fe3O4NPs was excellent compared to those of the well-established TiO2 micro-spheres. The enrichment protocol was extended for a second elution step facilitating the identification of additional phosphopep-tides. It further turned out that both types of amorphous TiO2 nanotubes provide qualitatively new physico-chemical features that are clearly advantageous for highly selective phosphopeptide enrichment. This has been confirmed experimentally resulting in substantial reduction of non-phosphorylated peptides in the enriched samples. In addition, TiO2NTs@Fe3O4NPs combine a high selectivity with ease of handling due to the superparamagnetic character of the material. The presented materials and performances are further promising for applications towards a whole range of other types of biomolecules to be treated in similar fashion.