The development of intelligent materials, in particular those showing the highly sensitive mechanoresponsive luminescence (MRL), is desirable but challenging. Here we report a design strategy for constructing high performance On–Off MRL materials by introducing nitrophenyl groups to molecules with aggregation-induced emission (AIE) characteristic. The on–off methodology employed is based on the control of the intersystem crossing (ISC) process. Experimental and theoretical investigations reveal that the nitrophenyl group effectively opens the nonradiative ISC channel to impart the high sensitivity and contrast On–Off behavior. On the other hand, the twisted AIE luminogen core endows enhanced reversibility and reduces the pressure required for the luminescence switching. Thin films can be readily fabricated from the designed materials to allow versatile applications in optical information recording and haptic sensing. The proposed design strategy thus provides a big step to expand the scope of the unique On–Off MRL family.
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