The presented study concerned up-converting core/shell type nanomaterials based on lanthanide(III) ions, Ln(III), doped orthoborates. The system studied composed of the GdBO3 doped with Yb3+/Tb3+ luminescent core ensured an effective cooperative sensitization up-conversion, resulting in a bright green luminescence. The silica coating process was performed by a modified Stöber method, which resulted in the formation of core-shell nanostructures, making them suitable for bioapplications. The nanophosphors and nanocomposites were obtained by various methods, such as co-precipitation in the presence of Triton X-100 and micelle synthesis with ethylenediaminetetraacetic acid (EDTA) as organic modifiers/surfactants. The synthesized nanomaterials were characterized with the use of powder X-ray diffraction (XRD), infrared light absorption with Fourier transform FT-IR spectra, transmission electron microscopy (TEM), up-conversion emission spectra under IR light, as well as excitation spectra, emission spectra and fluorescence lifetimes under UV light, and their photophysical properties were compared.