Due to its outstanding properties, diamond is considered as an ideal material for mechanical and electric applications at high temperatures, voltages, radiation, etc. It is known that femtosecond lasers exhibit extremely high precision and minimized thermal effect in material processing. In this study, a seed-free diamond pattern growth method was developed by patterning silicon substrates using a femtosecond laser before diamond deposition through laser-assisted combustion flame synthesis. The resolution of the diamond patterns reaches micro scales. Peak position, full width at half maximum (FWHM), and diamond quality parameter were calculated from Raman spectra. The mechanism of the seed-free diamond growth based on the femtosecond laser patterning was discussed. The influence of substrates surface roughness on the diamond nucleation and subsequent growth was studied, indicating that the nucleation density is proportional to the surface roughness.