The current study reports the use of silver (Ag) and samarium (Sm) as dopants to improve the properties of standard bioglass in terms of biological performance. This experiment considers thin films of doped bioglass obtained by pulsed laser deposition (PLD) and spin coating (SC). For both methods, some parameters were gradually varied, as the main objective was to produce a bioglass that could be used in biomedical fields. In order to study the morphology, the phase composition and other properties, the samples obtained were subjected to multiple analyses, such as thermal analysis, scanning electron microscopy (SEM), energy-dispersive X-ray spectroscopy (EDX), Fourier-transform infrared (FT-IR), Raman spectroscopy, and x-ray diffraction (XRD). Furthermore, the in vitro bioactivity of the samples, as assessed through simulated body fluid (SBF) immersion, as well as immunocytochemistry and evaluation of actin filaments, assessed through fluorescence microscopy, are reported. The results confirmed the formation of the designed vitreous target employed as the source of material in the PLD experiments only at sintering temperatures below 800 °C; this vitreous nature was preserved in the grown film as well. The presence of Ag and Ce dopants in the parent glassy matrix was validated for all stages, from powder, to target, to PLD/SC-derived coatings. Additionally, it was demonstrated that the surface topography of the layers can be adjusted by using substrates with different roughness or by modulating the processing parameters, such as substrate temperature and working pressure in PLD, rotation speed, and number of layers in SC. The developed material was found to be highly bioactive after 28 days of immersion in SBF, but it was also found to be a potential candidate for inhibiting the growth of Gram-negative bacteria and a suitable support for cell growth and proliferation.