The modulations of high/low-speed large-scale motions (H/L-SMs) on the turbulent/non-turbulent interface (TNTI) and turbulent entrainment are investigated in turbulent boundary layers via both experimental and numerical studies. The spanwise locations of large-scale motions can be locked by the spanwise heterogeneity, so the boundary layers over such a configuration are investigated first as an instructive case. In the engulfment process, it is found that irrotational ‘bubbles’ near the TNTI are more likely to originate from engulfment, while bubbles far from the TNTI could be produced by the local turbulence itself. Additionally, H-SMs are found to enhance the engulfment by the sweep flow. In the nibbling process, a competition relationship is observed: L-SMs induce stronger instantaneous ‘nibbling’ events by transporting more fluids towards the TNTI, while the H-SMs induced a more distorted TNTI. Consequently, the integral nibbling flux is greater above H-SMs. Furthermore, the explored mechanisms are verified to be insensitive to the wall shapes such as smooth and homogeneous roughness walls, which demonstrates that these modulations are universal for turbulent boundary layers. Finally, a conceptual modulation model is proposed to illustrate the entrainment process above the large-scale motions.