Epitaxial La0.7Ca0.3MnO3 (LCMO) thin films were prepared by thermal and excimer laser (EL) metal-organic deposition (MOD). Using simple thermal annealing (STA) at 800–1000°C, the LCMO films were well epitaxially grown on single-crystalline SrTiO3 substrates. When, using a KrF or an ArF excimer laser irradiation, the LCMO films were also epitaxially grown at a substrate temperature of 500°C. The films produced by STA exhibited metal–insulator transition temperatures T
p's ranging from 282 to 290 K while those obtained by EL irradiation had a T
p of approximately 205 K. For bolometric applications, the temperature coefficient of resistance (TCR) of the films was calculated. The LCMO films obtained by STA have a TCR of 8.5%/K at 228 K. On the other hand, using the EL irradiation, the TCR values are 5.8%/K at 165 K and 6.5%/K at 128 K for the KrF and ArF excimer lasers, respectively.