Amino carbon nanohorns (CNH–NH2) are covalently and non-covalently functionalized with tetrabenzoic acid porphyrin (H2P(CO2H)4) forming dispersible nanohybrids in aqueous solution; the nanohybrids are characterized by spectroscopy and electron microscopy. Photoinduced electron-transfer processes of the nanohybrids of carbon nanohorns in aqueous solution are revealed with time-resolved absorption and fluorescence measurements. From the observed fluorescence quenching of the H2P(CO2H)4 moieties by CNH–NH2, charge separation via the excited singlet state of the H2P moieties, generating radical cations localized in the H2P moieties and electrons trapped in CNH, is suggested. In the presence of methylviologen dication (MV2+) and a hole-shifting reagent, electron pooling is observed by the light-illumination of the H2P(CO2H)4 moieties in CNH–NH2 nanohybrids, suggesting that the electron generated by the charge-separation migrates to MV2+ in aqueous solution.