A method for depositing large grained polycrystalline GaAs on lattice mismatched substrates through controlled nucleation and selective growth is presented. The process was developed on Si wafers. Nucleation site formation began with nanolithography to create submicron holes in photoresist on Si. Ga metal was electrochemically deposited into the holes. Subsequent arsine anneals converted the gallium deposits into GaAs. Photoluminescence and electron diffraction verified conversion to GaAs. Metal-Organic Chemical Vapor Deposition (MOCVD) enlarged the seed crystals to coalescence without creating additional nucleation sites within the patterned field. Having successfully demonstrated the approach, subsequent work has been directed at lower cost, alternative ways to define initial nucleation sites, such as, microcontact lithography and direct decomposition of triethyl gallium to Ga metal in the MOCVD chamber.