In summary, this study unambiguously establishes the exceptional mechanosensitivity of chemo-mechanical coupling in diarylethene atropisomers, as evidenced through both computational and experimental methods. The F* value for the previously introduced M2 structure is 197 pN ± 12 pN as determined by SMFS. This value is lower than typically observed in other mechanically induced chemical reactions studied to date by SMFS, corroborating our previous indirect findings. Additionally and importantly, we introduce an intuitive 'lever-arm' effect that allows for the fine-tuning of the mechanical reactivity in diarylethene configurational mechanophores, leading to the development of a new mechanophore M3 which exhibits further increased mechanosensitivity with an F* value of 131 pN ± 4 pN. These atropisomeric diarylethene mechanophores also feature excellent thermal stability and are inherently photoinert, making them well-suited as molecular force probes with high specificity to mechanical stimuli. This study lays the groundwork for exploring the SMAR in this mechanistically distinct class of atropisomeric configurational mechanophores. It also paves the way for designing highly sensitive and irreversible mechanochemical processes that are crucial for understanding nanoscale mechanical behaviors in various synthetic and biological materials.