We present data on thin films of YBa2Cu3O7 (YBCO) and YBa2(Cu1−xFex)3O7 prepared by laser ablation using a sequence of targets, including Cu-deficient YBa2Cu2.4O7, CuO, and (CuO)1−y(FeO)y. This technique achieves mixing on an atomic scale. We find that stochiometric films, made using a combination of the Cudeficient target and CuO, have a sharp transition (width < 1K) near 90K although the Cu-deficient material alone has a broad transition at a lower Tc. We have achieved substitution of Fe on the Cu sites, using a sequence of the three targets for a range of Fe concentrations. Tc decreases nearly linearly with concentration and Tc → 0 near 15% Fe. The Tc suppression for the films is slightly less than the corresponding value obtained for bulk samples.