This study investigates the quantification of interfacial triboelectricity in inorganic-organic composite mechanoluminescent (ML) materials, which are promising for intelligent sensors, self-powered displays, and wearable devices. The authors propose a method to measure the triboelectric series between inorganic and organic phases, revealing that the ML intensity is positively correlated with the difference in the triboelectric series. This correlation is demonstrated through a series of composites, achieving a 20-fold increase in ML intensity by selecting appropriate inorganic-organic combinations. The study also confirms the role of interfacial triboelectricity in multi-interface systems, including inorganic phosphor-organic matrix and organic matrix-force applicator interfaces. The findings provide experimental evidence for the mechano-to-photon conversion mechanism and offer guidelines for designing high-efficiency ML materials. The work highlights the importance of interfacial triboelectricity in self-recoverable ML and its potential applications in advanced sensing and energy utilization.This study investigates the quantification of interfacial triboelectricity in inorganic-organic composite mechanoluminescent (ML) materials, which are promising for intelligent sensors, self-powered displays, and wearable devices. The authors propose a method to measure the triboelectric series between inorganic and organic phases, revealing that the ML intensity is positively correlated with the difference in the triboelectric series. This correlation is demonstrated through a series of composites, achieving a 20-fold increase in ML intensity by selecting appropriate inorganic-organic combinations. The study also confirms the role of interfacial triboelectricity in multi-interface systems, including inorganic phosphor-organic matrix and organic matrix-force applicator interfaces. The findings provide experimental evidence for the mechano-to-photon conversion mechanism and offer guidelines for designing high-efficiency ML materials. The work highlights the importance of interfacial triboelectricity in self-recoverable ML and its potential applications in advanced sensing and energy utilization.