Abstract Antimony (Sb) thin films are increasingly crucial in semiconductor technology due to their unique electronic and optical characteristics. Pulsed laser deposition (PLD) enhances their production by improving control over film microstructure and addressing uniformity challenges. The mechanical properties of Sb films, especially their behavior under mechanical stress and the associated twinning phenomena, are not well understood. This study employs nanoindentation and electron microscopy to investigate the mechanical properties and twinning behavior of Sb films deposited by PLD. Utilizing SEM and TEM, we analyze the structural changes these films undergo under stress, with a particular focus on deformation twinning, which critically affects their strength. Our findings confirm that deformation twinning, in particular, rhombohedral twinning plays a key role in determining the mechanical properties of Sb thin films. Nanoindentation reveals an activation volume of (2.75–3.85)b3 and a strain rate sensitivity of about 0.05 for Sb films. This research not only fills the existing knowledge gap about the mechanical behaviors of Sb thin films but also highlights the potential of PLD in producing high-quality films for high-performance applications, such as phase change materials, highlighting the transformative potential of PLD in tailoring the mechanical properties of thin films, crucial for next-generation electronic and optical devices.