Technological innovation is considered an important technical means to reduce carbon emissions and increase carbon removal. As two important aspects of carbon neutralization, there is little research on carbon neutralization in technological innovation. We utilized panel data to evaluate the spatial spillover effect of technological innovation on carbon neutrality via a dynamic spatial Durbin model and moderating effect model. We find that there are noticeable differences in the spillover effect of technological innovation on carbon neutrality from heterogeneous technological sources. The spatial impact of technological advancement on carbon neutrality is clearly defined by regional boundaries within 816 km. Foreign investments and introductions have a measurable moderating impact on the carbon deficit, whereas domestic-purchased technological innovation has a negligible impact. This study provides a basis for better utilizing technological innovation’s fundamental and crucial supporting role in the process of achieving carbon neutrality goals and low carbon development in China.