The existing mechanoluminesence has a single band. The 3P1→1S0 transition of Bi3+ ion can achieve an ultrabroadband emission in UV.Visible. However, the existing Bi3+ ion activated mechanoluminesence materials only emit blue light. To solve this problem, the UV.Visible.NIR ultrabroadband mechanoluminesence is realized in a multi-lattice garnet compound matrix, and its mechanoluminesent performance is regulated by the neighbor ion (i.e., Sc3+ ion) substitution strategy. The luminescence source is determined by steady-state fluorescence spectroscopy (at 465 nm, corresponding to the 3P1→1S0 transition of Bi3+ ion). The mechanism of mechanoluminesence is related to the persistent luminescence. The material defect distribution is obtained by thermoluminescence test, and the deep trap (>0.7 eV) contributes to the mechanoluminesence.