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A previously reported multistep hot filament chemical vapor deposition process for nucleating diamond directly on nickel substrates has been further refined to increase the nucleation density and improve the orientation of diamond films. The process employed heavy seeding of both 〈100〉 and 〈111〉 oriented single crystal Ni surfaces with diamond powders to enhance the nucleation density of diamond films. The deposition conditions were adjusted to allow for 〈100〉 and 〈111〉 orientations to grow on similarly oriented substrates to form nearly complete films with grain boundaries being eliminated. Thus, the technique holds promise for developing heteroepitaxial diamond films for microelectronics applications.