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Visible electrochemiluminescence (ECL) of singlet oxygen (1O2) from the dimeric 1Δgstate is a versatile and cost-efficient tool for sensing and imaging in various application fields such as biochemistry, pharmaceuticals, and material science. However, its implementation is hindered by weak emission and complex generation mechanisms. In this work, we enable a bright and switchable dimeric 1O2ECL through facile yet effective surface engineering strategies on a screen-printed carbon electrode in aqueous media. Specifically, we complement a stepwise potential procedure with a pre-cathodic process to switch on the anodic 1O2ECL and unravel how the in situelectrochemical pretreatments remarkably amplify the ECL intensity by modifying the surface oxygenates and promoting the 1O2-generating reactions. Additionally, ex situoxygen plasma treatment on the electrode surface, which switches off the 1O2ECL, further demonstrates the surface specificity of the 1O2ECL from another perspective. Leveraging these surface strategies, we establish a sensing capability of the 1O2ECL system with high sensitivity and selectivity toward tertiary amines. This work paves the way for translating a laboratory-scale 1O2-ECL system to portable and patternable sensing, imaging, and display applications.