Pt top contacts have been deposited by pulsed laser deposition (PLD) onto bare and tetradecylphosphate (TDP) self-assembled monolayer (SAM)-modified Nb-doped SrTiO3 (Nb-STO) substrates. For the SAM-modified substrates, electrochemical Cu deposition occurred only at the places where electrical shorts existed between the top contact and the substrate. A nearly perfect yield of top contacts without shorts was obtained, which shows the dense packing and robustness of the SAM. The SAM decreased the leakage current about 500 times compared to the bare substrate. Alkylphosphate SAMs on conducting metal oxide substrates can therefore be used as dielectric thin films for device fabrication.