Developing advanced and economically viable technologies for the capture and utilization of carbon dioxide (CO2) is crucial for sustainable energy production from fossil fuels. Converting CO2 into valuable chemicals and fuels is a promising approach to mitigate atmospheric CO2 levels. Among various methods, photocatalytic reduction stands out for its potential to reduce emissions and produce useful products. Here, novel perovskite ZnMoFeO3 (ZMFO) nanosheets are presented as promising semiconductor photocatalysts for CO2 reduction. Experimental results show that ZMFO has a narrow bandgap, exceptional visible light response, large specific surface area, high crystallinity, and various surface‐active sites, leading to an impressive photocatalytic CO2 reduction activity of 24.87 µmolg−1h−1 and strong stability. Theoretical calculations reveal that CO2 conversion into CO and CH4 on the ZMFO surface follows formaldehyde and carbine pathways. This study provides significant insights into designing innovative perovskite oxide‐based photocatalysts for economical and efficient CO2 reduction systems.