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Heteroepitaxial Zn-doped p-GaP was grown on (001) GaAs, (001) Si and (111) Si substrates by hydride vapor phase epitaxy for solar-driven photoelectrochemical applications of hydrogen generation by water splitting and CO2 reduction. Growth of GaP on Si was realized through the implementation of a low-temperature buffer layer, and the morphology and crystalline quality were enhanced by optimizing the precursor flows and pre-heating ambient substrate. The p-GaP/GaAs and p-GaP/Si samples were processed to photoelectrodes with an amorphous TiO2 coating for CO2 reduction and a combination of TiO2 layer and mesoporous tungsten phosphide catalyst for water splitting. P-GaP/GaAs with suitable Zn-doping concentration exhibited photoelectrochemical performance comparable to homoepitaxial p-GaP/GaP for water splitting and CO2 reduction. Degradation of photocurrent in p-GaP/Si photoelectrodes is observed in PEC water splitting due to the high density of defects arising from heteroepitaxial growth.