A novel approach for tailoring strained Pt model electrocatalysts using pulsed laser deposition is presented. The physical properties of Pt films grown on single-crystalline (100)- and (111)-oriented strontium titanate depend significantly on the various deposition parameters (e.g., fluence, temperature, background atmosphere, postannealing, and number of process steps), as revealed by scanning electron microscopy and X-ray studies. By properly selecting the deposition conditions, thin, epitaxial, and strained (100)- and (111)-oriented Pt films suitable as model electrodes can be prepared. Cyclic voltammetry measurements indicate that the strain in the Pt films changes significantly the Pt surface properties, such as the hydrogen underpotential deposition (H_upd) features. CO oxidation experiments demonstrate that the strain affects strongly also the position of the CO oxidation peak shifting it to more positive potentials. This might be attributed to a modification of the adsorption behavior of oxygenated species on the strained interface. This research clearly highlights the potential of using as-produced Pt film as model catalysts to study the effect of strain on electrocatalytic reactions while minimizing possible side effects connected to the common preparation methods for strained Pt catalysts, such as alloy formation, alloy leeching, or conductive support contributions.