Highly (001)-oriented (Pb0.76Ca0.24)TiO3 (PCT) thin films were grown on Pt/Ti/SiO2/Si substrates using a sol-gel process. The PCT film with a highly (001) orientation showed well-saturated hysteresis loops at an applied field of 800 kV/cm, with remanent polarization (P-r) and coercive electric field (E-c) values of 23.6 muC/cm(2) and 225 kV/cm, respectively. At 100 kHz, the dielectric constant and dielectric loss values of these films were 117 and 0.010, respectively. The leakage-current density of the PCT film was 6.15 x 10(-8)A/cm(2) at 5 V. The pyroelectric coefficient (p) of the PCT film was measured using a dynamic technique. At room temperature, the p values and figures-of-merit (F-D) of the PCT film were 185 muC/m(2)K and 1.79 x 10(-5) Pa-0.5, respectively.