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Electrocatalytic CO2 reduction technology is key to mitigating greenhouse gas emissions and the energy crisis. However, controlling the selectivity of CO2RR products at low overpotential remains a challenge. In this paper, we predicted five high-performance CO2RR electrocatalysts with different product-specific selectivities at the theoretical level based on the advantages of the compositional structure and the tunable pore size of 2D {\pi}-conjugated MOFs. In addition, through the reaction mechanism and electronic structure analysis, we found that the synergistic interaction between metal atoms and organic linkers of 2D MOFs can effectively regulate the electronic structure of the active center. Their pore size as well as the diversity of carbon materials can regulate the spin magnetic moments of the metal atoms, thus affecting the improvement of their catalytic performance. Meanwhile, the oxygen or carbon affinity of the catalyst surface determines the differences in the formation of key intermediates, which ultimately determines the reaction path and product selectivity. These insights we present will be useful for the development and design of highly active CO2RR electrocatalysts.