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Lone-pair electrons (LPEs) ns2 in subvalent 14 and 15 groups lead to highly anharmonic lattice and strong distortion polarization, which are responsible for the groups' outstanding thermoelectric and optoelectronic properties. However, their dynamic stereochemical role in structural and physical properties is still unclear. Here, by introducing pressure to tune the behavior of LPEs, we systematically investigate the lone-pair stereochemical role in a Bi2O2S. The gradually suppressed LPEs during compression show a nonlinear repulsive elect