Abstract: | CaRuO3 thin films with various thicknesses were synthesized by pulsed laser deposition respectively on SrTiO3 substrates with SrO‐ and TiO2‐termination. The microstructure of these films was studied by transmission electron microscopy. The results demonstrate that the CaRuO3 thin films grown on TiO2‐terminated substrates show quite uniform morphology, whilst they do the facet morphology when the substrates are SrO‐terminated. In addition, there is a 5∼7 unit‐cell‐thickness cubic CaRuO3 layer in the films grown on TiO2‐terminated substrates. The measured ferromagnetic hysteresis loop is attributed to the cubic CaRuO3 layer, which is supported by a first‐principles calculations. On the contrary, there is free of cubic CaRuO3 layer in samples grown on SrO‐terminated substrates. The crystallographic domains, the orientation relationship between domains and substrates and crystal defects in these films were studied as well. The different growth mechanism of CaRuO3 on SrO‐ and TiO2‐terminated SrTiO3 substrates may be correlated with the selective nucleation and growth. |