Single phase Tl2Ba2CaCu2O8 thin films have been deposited on single‐crystal LaAlO3 substrates, (100) orientation, via a two‐step deposition process. First, Ba‐Ca‐Cu‐O precursor films were deposited by metalorganic chemical vapor deposition (MOCVD) using barium, calcium, and copper‐tetramethyl‐heptanedionate, (tmhd)2, source materials under reduced pressure in an oxygen/argon atmosphere. Substrate temperatures were between 500 and 600 °C. Thallium was then incorporated by heating the films in a confined surface configuration with an unfired pellet of Tl2Ba2CaCu2Ox composition at 870 °C for 0.1 h. The resultant films (0.5–1 μm thick) showed a preferred orientation with the c axis normal to the substrate. The superconducting properties were characterized by resistance and mutual inductance versus temperature and by critical current measurements. Zero resistance temperatures as high as 98 K and Jc values close to 1×104 A/cm2 at 77 K were observed.