Laser-assisted atom probe tomography was used to investigate the nanostructure and composition of high-performance, ultra-hard Ti-Si-N nanocomposite films. However, the quality of data is heavily dependent on analysis conditions. In order to obtain reliable data from these, and other 'less conducting' specimens, the analysis parameter space was thoroughly investigated to optimize the mass resolution and hit multiplicity obtained in atom probe tomography. Geometric factors including tip radius and shank angle were found to play a significant role in mass resolution but had no apparent effect on the number of multiple hits observed. Increased laser energy led to a gradual increase in the number of single hits, but a modest improvement in mass resolution. The influence of other instrumental factors including detection rate and base temperature was investigated separately. Preliminary PLAP results are presented, and correlated with TEM analysis of the microstructure of the film.