The morphology of carbon nanotube (CNT) films is an important factor in the performance of CNT/silicon (CNT/Si) heterojunction solar devices. Films have generally been prepared via vacuum filtration from aqueous suspensions. Whilst this enables strong films to be formed quickly, they are highly disordered on the micron scale, with many charge traps and gaps forming in the films. It has been previously established that lowering the filtration speed enables more ordered films to be formed. The use of slow gravity filtration to improve the morphology of CNT films used in the CNT/Si device is reported here. It was found that slow filtration causes significant macroscale inhomogeneity in the CNT films, with concentrated thick regions, surrounded by larger thinner areas. By using atomic force microscopy (AFM), scanning electron microscopy (SEM), and polarised Raman spectroscopy, it was determined that there was no large improvement in directional organisation of the CNTs on the microscale. However, the films were found to be much smoother on the microscale, with arithmetic and root mean square average height deviation values roughly 3 times lower for slow-filtered films compared to fast-filtered films. A comparison was performed with CNT-Si solar cells fabricated with both slow and fast-filtered single-walled CNTs (SWCNT) films. It was found that slow filtration can produce similar photovoltaic results with thinner films. The results demonstrate that film morphology, even without improved CNT alignment, can lead to significant improvement in device performance in some applications. However, slow filtration did not form films of uniform light transmittance over an extended area, causing an increase in the variation in performance between individual devices compared to fast-filtered films.