The spectral sensitization of single-crystal p-GaP by semiconducting single-walled carbon nanotubes (s-SWCNT) via hole injection into the p-GaP valence band is reported. The results are compared to SWNCT sensitized n-type single-crystal substrates: TiO2, SnO2, and n-GaP. It was found that the sensitized photocurrents from CoMoCAT and HiPco s-SWCNTs were from a hole injection mechanism on all substrates, even when electron injection into the conduction band should be energetically favored. The results suggest an intrinsic p-type character of the s-SWCNTs surface films investigated in this work.