The osteogenic properties displayed by hybrid silica sol-gel materials make these compositions perfect candidates to be employed in bone tissue engineering applications. The present study aims to develop and characterize hybrid silica coatings, synthetized from mixtures between tetraethylorthosilicate (TEOS) and three different methyl-modified alkoxysilanes: trimethoxymethylsilane (MTMS), dimethyldiethoxylsilane (DMDES) and polydimethylsiloxane (PDMS). The comparison of the properties of these materials would allow to determinate which one is the best option to be applied onto metallic prosthesis for bone tissue application. After optimizing the synthesis parameters, the developed coatings were characterized using Fourier transform infrared spectrometry (FT-IR), 1 H and 29 Si solid state Nuclear Magnetic Resonance (1 H-NMR and 29 Si-MNR), cross-cut tests, contact angle measurements, optical profilometry, hydrolytic degradation tests and electrochemical impedance spectroscopy essays (EIS). Homogeneous and well-adhered coatings were obtained with the three methyl-modified reagents. However, different behaviours of metal protection against corrosion, hydrophilicity and degradation kinetics resulted depending on the initial precursor. The MTMS-based coating showed the highest hydrophilicity and degradation kinetics, properties that can lead to a greater bioactivity (Si release). While PDMS and DMDES-based coatings presented a higher barrier properties. From the physicochemical standpoint, all these materials presented interesting characteristics to be employed as coatings for biomedical applications.