Coal is the main energy source in China, with 4.5 billion metric tons of coal gangue accumulating near the mining areas in the process of coal mining. The objectives of the present study were to identify the health risks to children from soil pollution caused by coal gangue accumulation and to clarify the possible developmental neurotoxicity caused by this accumulation using zebrafish (Danio rerio) as a model. The results reveal that As and seven other heavy metals in soil samples from the gangue dumping area to the downstream villages exhibited distance-dependent concentration variations and posed substantial potential non-carcinogenic risks to local children. Additionally, soil leachate could affect the key processes of early neurodevelopment in zebrafish at critical windows, mainly including the alterations of cytoskeleton regulation (α1-tubulin), axon growth (gap43), neuronal myelination (mbp) and synapse formation (sypa, sypb, and psd95), eventually leading to hypoactivity in the zebrafish larvae. These findings suggest the possible health risks of soil pollution in the coal gangue stacking areas to children, particularly affecting their early neurodevelopment.