Zn1−xSmxO nanoparticles, with 0.00 ≤ x ≤ 0.10, were prepared using chemical co-precipitation method. The structure and morphology of the obtained samples were characterized using x-ray powder diffraction (XRD), transmission electron microscopy (TEM) and scanning electron microscopy (SEM), respectively. However, the mechanical properties were investigated via digital Vickers microhardness tester. Vickers microhardness measurements were carried out at different applied loads, varying between 0.5 and 10 N at dwell time 60 s on pressed discs of average thickness 3 mm. Hv decreased as the Sm-content increased up to 0.02 and then it increased for higher concentrations. Whereas, it increased as the applied load increased, revealing that the samples exhibited a reverse indentation size effect (ISE). The microhardness measurements were interpreted using various models such as Meyer’s law, Hays and Kendall (HK) approach, elastic/plastic deformation (EPD), proportional specimen resistance (PSR) and the indentation-induced cracking (IIC). Mechanical parameters such as Young’s modulus (E), yield strength (Y), fracture toughness (K) and brittleness index (B) were calculated as a function of x. The most adequate model for the true microhardness of these samples is IIC. It was found that the addition of Sm content enhanced the mechanical properties of the prepared samples after x = 0.02. Dielectric measurements were used to compute different parameters such as real and imaginary parts of the complex permittivity, dielectric loss (tan δ) and ac conductivity (σ
ac).