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Ammonia modified graphene-carbon nanotubes/continuous carbon fiber reinforced epoxy unidirectional multiscale composites (AMGNS-MWCNT/CFEP) were prepared by adding ammonia modified graphene and carbon nanotubes to an epoxy matrix to reduce agglomeration of carbon nanofillers in the epoxy matrix and improve composites properties. Fourier transform infrared spectroscopy (FTIR), scanning electron microscope (SEM), and universal testing machines were used to characterize the properties of carbon nanofillers, AMGNS-MWCNT/epoxy nanocomposites, and AMGNS-MWCNT/CFEP unidirectional composites. When the AMGNS-MWCNT content was 1.0 wt%, flexural strength, the flexural modulus and interlaminar shear strength of AMGNS-MWCNT/CFEP unidirectional composites reached the maximum value of 1520.3 MPa, 138.88 GPa, and 87.80 MPa, respectively, which were 12.5%, 9.42%, and 10.1% higher than that of carbon fiber reinforced epoxy unidirectional composites (CFEP). The synergistic mechanism of two carbon nanofillers in the matrix is discussed.