Electrochemiluminescence (ECL) of highly efficient and non-toxic carbon quantum dots (CQDs) plays an important role in immunoassays. However, the high absolute value of the excitation potential and poor controllability make precise detection of low levels difficult. In this work, novel CQDs with low excitation potential were reported to be used for the ultra-sensitive immunoassay of neuron-specific enolase (NSE). It is noteworthy that the narrow bandgap CQDs exhibit a trigger potential of −0.5 V and show excellent applicability of ECL signal at an excitation potential of −0.8 V. This property eliminates side reactions and electrode passivation and significantly improves ECL efficiency. Based on this, the magnetic zeolite-imidazole framework (MZIF) nanoreactor with co-reaction acceleration was employed as a carrier for the in-situ encapsulation of CQDs. The constrained-enhanced ECL sensor platform demonstrated the ability to achieve stable and controllable signal output. A sandwich-type biosensor was constructed by introducing copper sulfide (Cu7S4) as a dual-mechanism quencher, with NSE serving as the target analyte. Moreover, the electrochemical detection method based on the differential pulse voltammetry (DPV) properties of Cu7S4, was successfully validated against ECL. The sensors constructed on magnetic electrodes exhibited a bimodal signal output of ECL and DPV, encompassing a wide detection range (0.001 ng/mL − 500 ng/mL) and low detection limit (0.18 pg/mL for ECL and 0.15 pg/mL for DPV). This design offers a novel approach to understanding the efficient emission of carbon dots and provides a solution for the sensitive detection of biomarkers in clinical research.