GaN-based light-emitting diodes (LEDs) with various reactor pressures for GaN nucleation layers (NLs) have been grown on Si (111) substrates by metal-organic chemical vapor deposition.The influence of reactor pressure for GaN NLs on the properties of GaN-based LEDs grown on Si (111) substrates is investigated in detail. It is revealed that crack-free GaN films are grown on the Si (111) substrate. As the reactor pressure for GaN NLs increases from 200 to 600 Torr, the full width at half maximum values of the X-ray diffraction rocking curves for the GaN (0002) and (10-12) planes decrease from 480 to 351 arcsec, and 868 to 445 arcsec, respectively, and therefore the threading dislocation density is greatly reduced, which is confirmed by the cross-sectional transmission electron microscopy measurement. Subsequently, the relationship between the bending and annihilation for dislocations and the modes for GaN NL are elucidated. Meanwhile, the effect of reactor pressure for GaN NL on the mode of GaN NL is also systematically studied.Furthermore, the light output power of GaN-based LEDs with GaN NLs grown at reactor pressure of 500 Torr is greatly improved by 73.66% in comparison with that of GaN-based LEDs with GaN NLs grown at reactor pressure of 200 Torr. This work provides a new approach for achieving highly-efficient GaN-based LEDs on Si (111) substrates.