As a highly toxic aldehyde, acrolein is widely found in diet and environment, and can be produced endogenously, posing a serious threat to human health. Herein, we designed a novel fluorescent nanoplatform integrating carbon dots‑manganese dioxide (CDs-MnO2) and glutathione (GSH) for all-in-one sensing and removal of acrolein. By converting Mn4+ to free Mn2+, GSH inhibited the inner filter effect (IFE) of MnO2 nanosheets, and the Michael addition of acrolein with GSH inhibited the GSH-induced Mn4+ conversion, forming an “off-on-off” fluorescence response of CDs. The developed fluorescent nanoplatform exhibited high sensitivity (LOD was 0.067 μM) and selectivity for the simultaneous detection and removal of acrolein. The combination of CDs-MnO2 hydrogels with smartphones realized the point-of-care detection of acrolein, yielding satisfactory results (recovery rates varied between 97.01–104.65%, and RSD ranged from 1.42 to 4.16%). Moreover, the capability of the nanoplatform was investigated for on-site evaluating acrolein scavengers' efficacy, demonstrating excellent potential for practical application.